Natural and anthropogenic methane sources in New England

We have recently completed a methane emissions inventory for the New England region. Methane emissions were calculated to be 0.91 Tg yr^-1, with wetlands and landfills dominating all other sources. Wetlands are estimated to produce 0.33 Tg CH₄ yr^-1, of which 74% come from Maine. Active landfills emit an estimated 0.28 Tg CH₄ yr^-1, 60% of which are generated from twelve landfills. Although uncertainty in the estimate is greater, emissions from closed landfills are on the same order of magnitude as active landfills and wetlands; 0.25 Tg CH₄ yr^-1. Sources of moderate magnitude include ruminant animals (0.05 Tg CH₄ yr^-1) and residential wood combustion (0.03 Tg CH₄ yr^-1). Motor vehicles, natural gas, and wastewater treatment make only minor contributions. New England is heavily forested and the soil uptake of atmospheric methane in upland forests, 0.06 Tg CH₄ yr^-1, decreases emissions from soils by about 18%. Although uncertainties remain, our estimates indicate that even in a highly urbanized region such as New England, natural sources of methane make the single greatest contribution to total emissions, with state totals varying between 8% (Massachusetts) and 92% (Maine). Because emissions from only a few large landfills dominate anthropogenic sources, mitigation strategies focused on these discrete point sources should result in significant improvements in regional air quality. Current federal regulations mandate landfill gas collection at only the largest sites. Expanding recovery efforts to moderately sized landfills through either voluntary compliance or further regulations offers the best opportunity to substantially reduce atmospheric methane in New England. In the short term, however, the large contribution from closed, poorly regulated landfills may make the attribution of air quality improvements difficult. Mitigation efforts toward these landfills should also be a priority.     

Inventory of aerosol and sulphur dioxide emissions from India. Part II—biomass combustion

A spatially resolved biomass burning data set, and related emissions of sulphur dioxide and aerosol chemical constituents was constructed for India, for 1996–1997 and extrapolated to the INDOEX period (1998–1999). Sources include biofuels (wood, crop waste and dung-cake) and forest fires (accidental, shifting cultivation and controlled burning). Particulate matter (PM) emission factors were compiled from studies of Indian cooking stoves and from literature for open burning. Black carbon (BC) and organic matter (OM) emissions were estimated from these, accounting for combustion temperatures in cooking stoves. Sulphur dioxide emission factors were based on fuel sulphur content and reported literature measurements. Biofuels accounted 93% of total biomass consumption (577 MT yr⁻¹), with forest fires contributing only 7%. The national average biofuel mix was 56 : 21 : 23% of fuelwood, crop waste and dung-cake, respectively. Compared to fossil fuels, biomass combustion was a minor source of SO₂ (7% of total), with higher emissions from dung-cake because of its higher sulphur content. PM_2.5 emissions of 2.04 Tg yr⁻¹ with an “inorganic fraction” of 0.86 Tg yr⁻¹ were estimated. Biomass combustion was the major source of carbonaceous aerosols, accounting 0.25 Tg yr⁻¹ of BC (72% of total) and 0.94 Tg yr⁻¹ of OM (76% of total). Among biomass, fuelwood and crop waste were primary contributors to BC emissions, while dung-cake and forest fires were primary contributors to OM emissions. Northern and the east-coast India had high densities of biomass consumption and related emissions. Measurements of emission factors of SO₂, size resolved aerosols and their chemical constituents for Indian cooking stoves are needed to refine the present estimates.     

Inventory of aerosol and sulphur dioxide emissions from India: I—Fossil fuel combustion

A comprehensive, spatially resolved (0.25°×0.25°) fossil fuel consumption database and emissions inventory was constructed, for India, for the first time. Emissions of sulphur dioxide and aerosol chemical constituents were estimated for 1996–1997 and extrapolated to the Indian Ocean Experiment (INDOEX) study period (1998–1999). District level consumption of coal/lignite, petroleum and natural gas in power plants, industrial, transportation and domestic sectors was 9411 PJ, with major contributions from coal (54%) followed by diesel (18%). Emission factors for various pollutants were derived using India specific fuel characteristics and information on combustion/air pollution control technologies for the power and industrial sectors. Domestic and transportation emission factors, appropriate for Indian source characteristics, were compiled from literature. SO₂ emissions from fossil fuel combustion for 1996–1997 were 4.0 Tg SO₂ yr⁻¹, with 756 large point sources (e.g. utilities, iron and steel, fertilisers, cement, refineries and petrochemicals and non-ferrous metals), accounting for 62%. PM_2.5 emitted was 0.5 and 2.0 Tg yr⁻¹ for the 100% and the 50% control scenario, respectively, applied to coal burning in the power and industrial sectors. Coal combustion was the major source of PM_2.5 (92%) primarily consisting of fly ash, accounting for 98% of the “inorganic fraction” emissions (difference between PM_2.5 and black carbon+organic matter) of 1.6 Tg yr⁻¹. Black carbon emissions were estimated at 0.1 Tg yr⁻¹, with 58% from diesel transport, and organic matter emissions at 0.3 Tg yr⁻¹, with 48% from brick-kilns. Fossil fuel consumption and emissions peaked at the large point industrial sources and 22 cities, with elevated area fluxes in northern and western India. The spatial resolution of this inventory makes it suitable for regional-scale aerosol-climate studies. These results are compared to previous studies and differences discussed. Measurements of emission factors for Indian sources are needed to further refine these estimates.     

The characteristics of Asian-dust storms during 2000–2002: From the source to the sea

About 42 Asian-dust storms influenced the mainland and China during 2000–2002. Based on the Micaps meteorology data provided by China Meteorological Administration, the basic characteristics, including the source, movement route and influenced areas were studied for each case. It was shown that about 70% Asian-dust storms that influence China came from Mongolia, and were strengthened during the way from west to east. In 2000–2002, there was about 63.9% Asian-dust weather that might have affected China seas through three different routes. The probability is affecting the Bohai Sea was 27.4%, the Yellow Sea 30.9%, the East China Sea 12.3%, the Korea Channel 20.2% and the Japan Sea 9.2%. Annual dry deposition flux to the Yellow Sea was about 0.13 g m⁻² d⁻¹, and in spring was ∼0.20 g m⁻² d⁻¹. The total amount of dry deposition to the Yellow Sea was ∼17.9 Tg yr⁻¹.     

Modelling base cations in Europe—sources,transport and deposition of calcium

The deposition of the base cations calcium, magnesium and potassium from the atmosphere needs to be quantified in the calculation of the total deposited acidity in the critical loads approach. Of these base cations, calcium has been found to be the most important in terms of mass deposited. However, the sources of calcium to the atmosphere are not well understood. Recently, the first spatially disaggregated inventory of industrial calcium emissions for Europe was presented by Lee and Pacyna (1998) who estimated a total European emission of 0.7–0.8 Mt yr^-1. However, it is thought that wind blown dust from soils contributes a substantial fraction to the deposition of calcium. In this work, the source strength of calcium from arid regions within the EMEP modelling domain was estimated using the global mineral dust emission data base of Tegen and Fung (1994) and an estimation of the calcium content of soils. This results in a “natural” calcium emission of 6 Mt yr^-1. A long-range transport model, TRACK, was used to calculate the wet and dry deposition of calcium arising from these industrial and natural sources to the UK which resulted in a total deposition of 29–30 kt yr^-1. Of this annual deposition, 0.6–0.7 kt arises from cement manufacturing, 0.02–0.03 kt from iron and steel manufacturing, 0.8–0.83 kt from a large point source power generation, and 28 kt from power generation from a small boiler plant. The natural emissions of calcium from arid regions result in a deposition of calcium to the UK of 0.5 kt yr^-1. The measured wet deposition of calcium to the UK is 89 kt yr^-1 and the estimated dry deposition 14 kt yr^-1. The short-fall in the modelled deposition of calcium is thus of the order of 70 kt yr^-1, which is suggested to arise from wind-blown dust from agricultural land in the UK and mainland Europe. The estimated emissions, and thus modelled deposition are rather uncertain, such that estimating deposition of calcium attributable to agricultural soil emissions by differencing has a large uncertainty. However, this is the first such study of its kind for Europe and represents a first step towards understanding the sources of calcium and their contribution to mitigating deposited acidity from acidifying pollutants such as sulphur dioxide, nitrogen oxides and ammonia.     

Secondary organic aerosol importance in the future atmosphere

In order to investigate the secondary organic aerosol (SOA) response to changes in biogenic volatile organic compounds (VOC) emissions in the future atmosphere and how important will SOA be relative to the major anthropogenic aerosol component (sulfate), the global three-dimensional chemistry/transport model TM3 has been used. Emission estimates of biogenic VOC (BVOC) and anthropogenic gases and particles from the literature for the year 2100 have been adopted.According to our present-day model simulations, isoprene oxidation produces 4.6 Tg SOA yr⁻¹, that is less than half of the 12.2 Tg SOA yr⁻¹ formed by the oxidation of other BVOC. In the future, nitrate radicals and ozone become more important than nowadays, but remain minor oxidants for both isoprene and aromatics. SOA produced by isoprene is estimated to almost triple, whereas the production from other BVOC more than triples. The calculated future SOA burden change, from 0.8 Tg at present to 2.0 Tg in the future, is driven by changes in emissions, oxidant levels and pre-existing particles. The non-linearity in SOA formation and the involved chemical and physical feedbacks prohibit the quantitative attribution of the computed changes to the above-mentioned individual factors. In 2100, SOA burden is calculated to exceed that of sulfate, indicating that SOA might become more important than nowadays. These results critically depend on the biogenic emissions and thus are subject to the high uncertainty associated with these emissions estimated due to the insufficient knowledge on plant response to carbon dioxide changes. Nevertheless, they clearly indicate that the change in oxidants and primary aerosol caused by human activities can contribute as much as the change in BVOC emissions to the increase of the biogenic SOA production in the future atmosphere.     

A revised estimate of copper emissions from road transport in UNECE-Europe and its impact on predicted copper concentrations

Comparisons of measured and model-predicted atmospheric copper concentrations show a severe underestimation of the observed concentrations by the models. This underestimation may be (partly) due to underestimated emissions of copper to air. Since the phase out of asbestos brake lining material, the composition of brake lining material has changed and may contain up to ∼15% copper. This makes brake wear from vehicles potentially an important source of atmospheric (particulate) copper concentrations. In this paper, we reassess the copper emissions due to exhaust emissions and brake wear from road transport. Overall, our reassessments result in an estimate of total copper emission to air in UNECE-Europe of 4.0–5.5 ktonnes yr⁻¹, which is substantially higher than the previous estimate of 2.8 ktonnes yr⁻¹. Copper concentrations over Europe are calculated with the LOTOS-EUROS model using the revised emission data as model input. The results show that the revised emission estimates are a major step towards gap closure of predicted versus observed copper concentrations in ambient air. Brake wear emissions may be responsible for 50–75% of the total copper emissions to air for most of Western Europe. The hypothesis that road transport is an important source of copper emissions is tested and confirmed by (1) reviewing available literature data of chemically speciated PM data from road tunnel studies and (2) the gradient observed in copper concentrations from ambient PM monitoring going from rural sites to street stations. The literature review and observational data suggest that the majority of the emitted PM10 brake wear particles is in the PM2.5–10 size range. The results of this study indicate that modification of brake lining composition is an important mitigation option to reduce copper exposure of the population in Western Europe.     

Historical deposition of mercury and selected trace elements to high-elevation National Parks in the Western U.S. inferred from lake-sediment cores

Atmospheric deposition of Hg and selected trace elements was reconstructed over the past 150 years using sediment cores collected from nine remote, high-elevation lakes in Rocky Mountain National Park in Colorado and Glacier National Park in Montana. Cores were age dated by ²¹⁰Pb, and sedimentation rates were determined using the constant rate of supply model. Hg concentrations in most of the cores began to increase around 1900, reaching a peak sometime after 1980. Other trace elements, particularly Pb and Cd, showed similar post-industrial increases in lake sediments, confirming that anthropogenic contaminants are reaching remote areas of the Rocky Mountains via atmospheric transport and deposition. Preindustrial (pre-1875) Hg fluxes in the sediment ranged from 5.7 to 42 μg m^?2 yr^?1 and modern (post-1985) fluxes ranged from 17.7 to 141 μg m^?2 yr^?1. The average ratio of modern to preindustrial fluxes was 3.2, which is similar to remote lakes elsewhere in North America. Estimates of net atmospheric deposition based on the cores were 3.1 μg m^?2 yr^?1 for preindustrial and 11.7 μg m^?2 yr^?1 for modern times. Current-day measurements of wet deposition range from 5.0 to 8.6 μg m^?2 yr^?1, which are lower than the modern sediment-based estimate of 11.7 μg m^?2 yr^?1, perhaps owing to inputs of dry-deposited Hg to the lakes.     

Air–water exchange fluxes of polycyclic aromatic hydrocarbons in the tropical coast,Taiwan

Air–water exchange fluxes of polycyclic aromatic hydrocarbons (PAHs) were simultaneously measured in air and water samples from two sites on the Kenting coast, located at the southern tip of Taiwan, from January to December 2010. There was no significant difference in the total PAH (t-PAH) concentrations in both gas and dissolved phases between these two sites due to the less local input which also coincided to the low levels of t-PAH concentration; the gas and dissolved phases averaged 1.29 ± 0.59 ng m^?3 and 2.17 ± 1.19 ng L^?1 respectively. The direction and magnitude of the daily flux of PAHs were significantly influenced by wind speed and dissolved PAH concentrations. Individual PAH flux ranged from 627 ng m^?2 d^?1 volatilization of phenanthrene during the rainy season with storm–water discharges raising dissolved phase concentration, to 67 ng m^?2 d^?1 absorption of fluoranthene during high wind speed periods. Due to PAH annual fluxes through air–water exchange, Kenting seawater is a source of low molecular weight PAHs and a reservoir of high molecular weight PAHs. Estimated annual volatilization fluxes ranged from 7.3 μg m^?2 yr^?1 for pyrene to 50 μg m^?2 yr^?1 for phenanthrene and the absorption fluxes ranged from ?2.6 μg m^?2 yr^?1 for chrysene to ?3.5 μg m^?2 yr^?1 for fluoranthene.     

Impact of mercury emissions from historic gold and silver mining: Global modeling

We compare a global model of mercury to sediment core records to constrain mercury emissions from the 19th century North American gold and silver mining. We use information on gold and silver production, the ratio of mercury lost to precious metal produced, and the fraction of mercury lost to the atmosphere to calculate an a priory mining inventory for the 1870s, when the historical gold rush was at its highest. The resulting global mining emissions are 1630 Mg yr^?1, consistent with previously published studies. Using this a priori estimate, we find that our 1880 simulation over-predicts the mercury deposition enhancements archived in lake sediment records. Reducing the mining emissions to 820 Mg yr^?1 improves agreement with observations, and leads to a 30% enhancement in global deposition in 1880 compared to the pre-industrial period. For North America, where 83% of the mining emissions are located, deposition increases by 60%. While our lower emissions of atmospheric mercury leads to a smaller impact of the North American gold rush on global mercury deposition than previously estimated, it also implies that a larger fraction of the mercury used in extracting precious metals could have been directly lost to local soils and watersheds.     

Global atmospheric emission inventory of polycyclic aromatic hydrocarbons (PAHs) for 2004

The global atmospheric emissions of the 16 polycyclic aromatic hydrocarbons (PAHs) listed as the US EPA priority pollutants were estimated using reported emission activity and emission factor data for the reference year 2004. A database for emission factors was compiled, and their geometric means and frequency distributions applied for emission calculation and uncertainty analysis, respectively. The results for 37 countries were compared with other PAH emission inventories. It was estimated that the total global atmospheric emission of these 16 PAHs in 2004 was 520 giga grams per year (Gg y^?1) with biofuel (56.7%), wildfire (17.0%) and consumer product usage (6.9%) as the major sources, and China (114 Gg y^?1), India (90 Gg y^?1) and United States (32 Gg y^?1) were the top three countries with the highest PAH emissions. The PAH sources in the individual countries varied remarkably. For example, biofuel burning was the dominant PAH source in India, wildfire emissions were the dominant PAH source in Brazil, while consumer products were the major PAH emission source in the United States. In China, in addition to biomass combustion, coke ovens were a significant source of PAHs. Globally, benzo(a)pyrene accounted for 0.05% to 2.08% of the total PAH emission, with developing countries accounting for the higher percentages. The PAH emission density varied dramatically from 0.0013 kg km^?2 y in the Falkland Islands to 360 kg km^?2 y in Singapore with a global mean value of 3.98 kg km^?2 y. The atmospheric emission of PAHs was positively correlated to the country's gross domestic product and negatively correlated with average income. Finally, a linear bivariate regression model was developed to explain the global PAH emission data.     

Fire and biofuel contributions to annual mean aerosol mass concentrations in the United States

We estimate the contributions from biomass burning (summer wildfires, other fires, residential biofuel, and industrial biofuel) to seasonal and annual aerosol concentrations in the United States. Our approach is to use total carbonaceous (TC) and non-soil potassium (ns-K) aerosol mass concentrations for 2001–2004 from the nationwide IMPROVE network of surface sites, together with satellite fire data. We find that summer wildfires largely drive the observed interannual variability of TC aerosol concentrations in the United States. TC/ns-K mass enhancement ratios from fires range from 10 for grassland and shrub fires in the south to 130 for forest fires in the north. The resulting summer wildfire contributions to annual TC aerosol concentrations for 2001–2004 are 0.26 μg C m⁻³ in the west and 0.14 μg C m⁻³ in the east; Canadian fires are a major contributor in the east. Non-summer wildfires and prescribed burns contribute on an annual mean basis 0.27 and 0.31 μg C m⁻³ in the west and the east, highest in the southeast because of prescribed burning. Residential biofuel is a large contributor in the northeast with annual mean concentration of up to 2.2 μg C m⁻³ in Maine. Industrial biofuel (mainly paper and pulp mills) contributes up to 0.3 μg C m⁻³ in the southeast. Total annual mean fine aerosol concentrations from biomass burning average 1.2 and 1.6 μg m⁻³ in the west and east, respectively, contributing about 50% of observed annual mean TC concentrations in both regions and accounting for 30% (west) and 20% (east) of total observed fine aerosol concentrations. Our analysis supports bottom-up source estimates for the contiguous United States of 0.7–0.9 Tg C yr⁻¹ from open fires (climatological) and 0.4 Tg C yr⁻¹ from biofuel use. Biomass burning is thus an important contributor to US air quality degradation, which is likely to grow in the future.     

Tropospheric halocompounds and nitrous oxide monitored at a remote site in the Mediterranean

Analysis of time series and trends of nitrous oxide (N₂O) and halocompounds weekly monitored at the Mediterranean island of Lampedusa are discussed. Atmospheric N₂O levels showed a linear upward growth rate of 0.78 ppb yr^?1 and mixing ratios comparable with Northern Hemisphere global stations. CFC-11 and CFC-12 time series displayed a decline consistent with their phase-out. Chlorofluorocarbons (CFCs) replacing compounds and SF₆ exhibited an increasing temporal behaviour. The most rapid growth rate was recorded for HFC-134a with a value of 9.6% yr^?1. The industrial solvents CCl₄ and CH₃CCl₃, banned by the Montreal Protocol, showed opposite trends. While CH₃CCl₃ reported an expected decay of ?1.8 ppt yr^?1, an increasing rate of 5.7 ppt yr^?1 was recorded for CCl₄ and it is probably related to its relatively long lifetime and persisting emissions. Chlorinated halomethanes showed seasonality with a maximum in early April and a minimum at the end of September. Halon-1301 and Halon-1211 displayed a decreasing trend consistent with industry emission estimates.An interspecies correlation analysis gave positive high correlations between HCFC-22 and HFC-134a (+0.84) highlighting the common extensive employment as refrigerants. Sharing sources inferred the high coupling between CH₃Cl and CH₃Br (+0.73) and between CHCl₃ and CH₂Cl₂ (+0.77). A singular strong relationship (+0.55) between HFC-134a and CH₃I suggested the influence of an unknown anthropogenic source of CH₃I.Constraining of source and sink distribution was carried out by transport studies. Results were compared with the European Environment Agency (EEA) emission database. In contrast with the emission database results, our back trajectory analysis highlighted the release of large amounts of HFC-134a and SF₆ from Eastern Europe. Observations also showed that African SF₆ emissions may be considerable. Leakages from SF₆ insulated electrical equipments located in the industrialized Northern African areas justify our observations.     

Modelling atmospheric mercury transport and deposition across Europe and the UK

There are inadequate measurements of surface ambient concentrations of mercury species and their deposition rates for the UK deposition budget to be characterized. In order to estimate the overall mercury flux budget for the UK, a simple long-term 1D Lagrangian trajectory model was constructed that treats emissions (1998), atmospheric transformation and deposition across Europe. The model was used to simulate surface concentrations of mercury and deposition across Europe at a resolution of 50 km×50 km and across the UK at 20 km×20 km. The model appeared to perform adequately when compared with the few available measurements, reproducing mean concentrations of elemental gaseous mercury at particular locations and the magnitude of regional gradients. The model showed that 68% of the UK's mercury emissions are exported and 32% deposited within the UK. Of deposition to the UK, 25% originates from the Northern Hemisphere/global background, 41% from UK sources and 33% from other European countries. The total mercury deposition to the UK is in good agreement with other modelling, 9.9 tonne yr⁻¹ cf. 9.0 tonne yr⁻¹, for 1998. However, the attribution differs greatly from the results of other coarser-scale modelling, which allocates 55% of the deposition to the UK from UK sources, 4% from other European countries and 60% from the global background atmosphere. The model was found to be sensitive to the speciation of emissions and the dry deposition velocity of elemental gaseous mercury. The uncertainties and deficiencies are discussed in terms of model parameterization and input data, and measurement data with which models can be validated. There is an urgent requirement for measurements of removal terms, concentrations, and deposition with which models can be parameterized and validated.     

An industrial emissions inventory of calcium for Europe

The base cations calcium, magnesium and potassium, have been observed to be declining in air and precipitation in both Europe and North America. There is good evidence that this is the result of declining emissions of fly ash from industrial plant, as a result of increased abatement and industrial decline. This may have the effect of offsetting the effects of declines in acidic emissions, in terms of net deposited acidity. In order to reconcile source strengths of base cations, an industrial emissions inventory of calcium, the dominant base cation in air and precipitation, has been compiled. The main sources identified were: cement plants; iron and steel plants; and coal combustion from both large and small boilers. The overall emission was calculated to be between approximately 750 and 800 ktonnes Ca yr^-1. The dominant source was coal combustion from domestic and small boilers. Of the point sources, cement production dominated over coal combustion, and iron and steel plant. The emission factors used are very uncertain, which gives the inventory a large uncertainty. Furthermore, the emissions are compiled on a base year of 1990, and large changes have taken place in the industrial structuring of the largest contributing countries. Despite the uncertainties, the compilation of the inventory represents a vital first step in understanding the sources of deposited calcium and its effect on net deposited acidity.     

Emissions of volatile fatty acids from feed at dairy facilities

Recent studies suggest that dairy operations may be a major source of non-methane volatile organic compounds in dairy-intensive regions such as Central California, with short chain carboxylic acids (volatile fatty acids or VFAs) as the major components. Emissions of four VFAs (acetic acid, propanoic acid, butanoic acid and hexanoic acid) were measured from two feed sources (silage and total mixed rations (TMR)) at six Central California Dairies over a fifteen-month period. Measurements were made using a combination of flux chambers, solid phase micro-extraction fibers coupled to gas chromatography mass spectrometry (SPME/GC–MS) and infra-red photoaccoustic detection (IR-PAD for acetic acid only). The relationship between acetic acid emissions, source surface temperature and four sample composition factors (acetic acid content, ammonia-nitrogen content, water content and pH) was also investigated. As observed previously, acetic acid dominates the VFA emissions. Fluxes measured by IR-PAD were systematically lower than SPME/GC–MS measurements by a factor of two. High signals in field blanks prevented emissions from animal waste sources (flush lane, bedding, open lot) from being quantified. Acetic acid emissions from feed sources are positively correlated with surface temperature and acetic acid content. The measurements were used to derive a relationship between surface temperature, acetic acid content and the acetic acid flux. The equation derived from SPME/GC–MS measurements predicts estimated annual average acetic acid emissions of (0.7 + 1/?0.4) g m^?2 h^?1 from silage and (0.2 + 0.3/?0.1) g m^?2 h^?1 from TMR using annually averaged acetic acid content and meteorological data. However, during the summer months, fluxes may be several times higher than these values.     

Historical changes in atmospheric nitrogen deposition to Cape Cod,Massachusetts, USA

We reconstructed the historical trends in atmospheric deposition of nitrogen to Cape Cod, Massachusetts, from 1910 to 1995 by compiling data from literature sources, and adjusting the data for geographical and methodological differences. The reconstructed data suggest that NO₃-N wet deposition to this region increased from a low of 0.9 kg N ha⁻¹ yr⁻¹ in 1925 to a high of approximately 4 kg N ha⁻¹ yr⁻¹ around 1980. The trend in NO₃-N deposition has remained since the early 1980s at around 3.6 kg N ha⁻¹ yr⁻¹. In contrast, NH₄-N wet deposition decreased from more than 4 kg N ha⁻¹ yr⁻¹ in the mid 1920s to about 1.5 kg N ha⁻¹ yr⁻¹ from the late-1940s until today. Emissions of NO_x-N in the Cape Cod airshed increased at a rate of 2.1 kg N ha⁻¹ per decade since 1910, a rate that is an order of magnitude higher than NO₃-N deposition. Estimates of NH₃ emissions to the northeast United States and Canada have decreased slightly throughout the century, but the decrease in reconstructed N-NH₄⁺ deposition rates does not parallel emissions estimates. The trend in reconstructed total nitrogen deposition suggests an overall increase through the century at a rate of 0.26 kg N ha⁻¹ per decade. This overall increase in deposition may expose coastal forests to rates of nitrogen addition that, if exceeded, could induce nitrogen saturation and increase nitrogen loads to adjoining estuaries.     

Density of foliage mass and area in the boreal forest cover in Finland,with applications to the estimation of monoterpene and isoprene emissions

The distribution of the density of foliage mass and area in forest canopies throughout Finland (60–70°N) were determined on the basis of the permanent sample plots used in the Finnish National Forest Inventory. These parameters were linked to the long-term monthly mean air temperatures for 1961–1990, which had been converted to hourly temperature and radiation values with the help of a weather simulator in order to calculate the spatial distribution of mean yearly emissions of monoterpene and isoprene over Finland. The mean total density of foliage mass in southern Finland (60°⩽latitude<65°N) was around 500 g m⁻², equivalent to 4–5 m² of total foliage area per m² of land area. In northern Finland (65°⩽latitude<70°N), the maximum values remained below 200–300 g m⁻², or 2–3 m² m⁻². The highest values were achieved in forests dominated by mature Norway spruces. The higher temperatures and longer growing season in southern Finland led to greater emissions than in the rest of the country. Total annual emissions of monoterpene were 1070 kg km⁻² yr⁻¹ in southern Finland and 460 kg km⁻² yr⁻¹ in the north, and those of isoprene from Norway spruce canopies 150 and 40 kg km⁻² yr⁻¹, respectively.     

Estimation of wind blown dust emissions in Europe and its vicinity

The assessment of the wind blown dust emission for Europe and selected regions of North Africa and Southwest Asia was carried out using a mesoscale model. The mesoscale model was parameterized based on the current literature review. The model provides data on PM₁₀ emission from several dust reservoirs (anthropogenic, agriculture, semi- and natural) with spatial resolution of 10 × 10 km and temporal resolution of 1 h. The spatial variability of PM₁₀ emission depends on soil texture, land cover/land use as well as meteorological conditions. Lands covered with water or permanently wet were excluded from the model. The land covered with vegetation is treated as dust reservoir whose dust emission capacity depends on the type of vegetation and cover. The dust reservoirs are divided into reservoirs with stable and unstable surface. The changes of emission in time depend on meteorological parameters.The wind blown dust emission should be treated as a non-continuous spatio-temporal process. The emissions are estimated with high uncertainty. The estimated PM₁₀ yearly total load emitted by wind from the European territory is highly differentiated in space and time and is equal to 0.74 Tg. The total load of PM₁₀ emitted by wind from North African and Southwest Asian land surface located in the vicinity of European boundaries is assessed as nearly 50% (0.43 Tg) of the total load estimated for the whole Europe.The average yearly PM₁₀ emission factor for Europe was estimated at 0.139 Mg km^?2.The PM₁₀ emission from agricultural areas is estimated at 52% of the total wind blown emission from the domain of the European Union project “Improving and applying methods for the calculation of natural and biogenic emissions and assessment of impacts to the air quality” - NatAir.PM₁₀ emission factor for natural areas of Europe is estimated at 0.021 Mg km^?2. Appropriate factors for agricultural areas and anthropogenic areas are 0.157 Mg km^?2 and 0.118 Mg km^?2, respectively. The latter two factors are probably underestimated due to omitting in the model of other dust emission mechanisms than aeolian erosion.     

Atmospheric methyl chloride

There are about 5 Tg of methyl chloride in the Earth’s atmosphere making it one of the largest reservoirs of gas-phase chlorine. We discuss the time series of global measurements taken over the last 16 yr at seven locations distributed among the polar, middle, and tropical latitudes of both hemispheres (1981–1997). Measurements were also taken at 20 more sites between 1987 and 1989. The vertical distribution was measured during campaign experiments in the Arctic, Western Atlantic, and over Brazil. Small, mostly decreasing trends are observed, showing that on average, there was 4% less methyl chloride during the last three years (1994–1996) than there was in the first three years (1985–1987) of the experiment. The latitudinal variation is marked by highest concentrations in the tropics and lowest in the polar regions. Sites representing inland locations show higher concentrations, suggesting continental sources, mostly confined to the tropics. There are seasonal variations at various latitudes that can be explained mostly by the cycles of OH radicals, which are the dominant removal process for methyl chloride in the atmosphere. Based on these data, the expected emissions can be calculated at the polar, middle, and tropical latitudes represented by the six long-term primary sites. Using a photochemical model of OH, we estimate that a global source of about 3.7 Tg yr^-1 of methyl chloride is needed to explain the observed concentrations. Other removal processes have been identified that may add to this estimate of the global annual emissions. The results further establish that some 85% of the emissions must come from the half of the earth’s surface between 30°S and 30°N, representing tropical and sub-tropical latitudes. Small emissions are estimated for the middle latitudes, and no emissions are expected from the polar regions.