A novel approach to peatlands as archives of total cumulative spatial pollution loads from atmospheric deposition of airborne elements complementary to EMEP data: priority pollutants (Pb, Cd, Hg).

A novel approach to using peatlands for assessment of cumulative contributions from long-range transport of pollutants (LRTP) - airborne trace elements - to spatial pollution was exemplified in evaluating retrospective atmospheric deposition of priority pollutants (Pb, Cd, Hg) in peat bogs in Norway in areas minor affected by local sources of pollution and in NW Poland located on the way of possible LRTP from Poland to Norway. Peat from the corresponding 14C-dated layers of five ombrotrophic bogs in each country, was analysed for trace element contents. Pollutant concentrations/load distribution along the peat profiles related to bulk density has given a clear evidence of uneven density-dependent temporal vertical migration of all studied elements that distorts the chronology of their deposition. Much higher loads of Pb, Cd and Hg in southern Norwegian bogs than in bogs located in NW Poland proved transboundary transport from neighbouring highly industrialized European countries to be much more significant contributor to high deposition of the priority pollutants in this area and rather excludes LRTP from Poland as a major source of total land pollution in southernmost Norway. The study showed excellent applicability of peat bogs for the exact assessment of retrospective cumulative pollutant loads from LRTP, but not for the identification of deposition chronology. Combining the use of ombrotrophic peat bogs as tools for retrospective monitoring of cumulative land pollution with airborne elements with current LRTP data within the Cooperative Programme for Monitoring and Evaluation of the Long-Range Transmission of Air Pollutants in Europe (EMEP) may provide a complete reliable picture of the effect of anthropogenic emissions on soil quality and create a foundation of optimum environmental policy and activities in this field.

Trace elements and polychlorinated biphenyls (PCBs) in terrestrial compartments of Svalbard, Norwegian Arctic.

Despite being a remote location, the Arctic is a major receptor for anthropogenic pollution transported from the mid-latitudes. Vegetation and underlying organic soils in the Norwegian Arctic, Svalbard were used to study the occurrences of polychlorinated biphenyls (PCBs) and trace elements. In this study, current concentrations of PCBs and trace elements, namely, Al, As, Cd, Cr, Cu, Fe, Hg, Mn, Ni, Pb, S, Sb, U and Zn in the terrestrial compartments of Svalbard are presented. Samples were collected from Adventdalen near Longyearbyen and from areas in proximity to Ny-Ålesund. There was significant variability in soil organic matter (SOM) among the soils analysed (5.0%-72.1%), with the highest values detected in Ny-Ålesund. The concentrations of Al, As, Cr Cu, Fe, Pb and Ni were associated with the geology of the local bedrock. The concentrations of all elements, except for Cd, Hg and Zn, were higher in soils than those in the overlying vegetation layers. Mean concentrations of ∑PCBs were significantly higher in vegetation (6.90 ±â€¯0.81 ng g-1 dw) than the underlying organic soils (3.70 ±â€¯0.36 ng g-1 dw). An inverse correlation of PCBs with the elements originating from the local bedrock indicated that their concentrations were potentially impacted by atmospheric deposition. PCBs and Cd were strongly associated, proposing a potential concomitant source of origin in Svalbard. Concentrations of PCBs and trace elements measured herein were below the proposed guidelines for Norwegian soil quality.

Modelling spatial patterns of correlations between concentrations of heavy metals in mosses and atmospheric deposition in 2010 across Europe.

BACKGROUND: This paper aims to investigate the correlations between the concentrations of nine heavy metals in moss and atmospheric deposition within ecological land classes covering Europe. Additionally, it is examined to what extent the statistical relations are affected by the land use around the moss sampling sites. Based on moss data collected in 2010/2011 throughout Europe and data on total atmospheric deposition modelled by two chemical transport models (EMEP MSC-E, LOTOS-EUROS), correlation coefficients between concentrations of heavy metals in moss and in modelled atmospheric deposition were specified for spatial subsamples defined by ecological land classes of Europe (ELCE) as a spatial reference system. Linear discriminant analysis (LDA) and logistic regression (LR) were then used to separate moss sampling sites regarding their contribution to the strength of correlation considering the areal percentage of urban, agricultural and forestry land use around the sampling location. After verification LDA models by LR, LDA models were used to transform spatial information on the land use to maps of potential correlation levels, applicable for future network planning in the European Moss Survey. RESULTS: Correlations between concentrations of heavy metals in moss and in modelled atmospheric deposition were found to be specific for elements and ELCE units. Land use around the sampling sites mainly influences the correlation level. Small radiuses around the sampling sites examined (5 km) are more relevant for Cd, Cu, Ni, and Zn, while the areal percentage of urban and agricultural land use within large radiuses (75-100 km) is more relevant for As, Cr, Hg, Pb, and V. Most valid LDA models pattern with error rates of < 40% were found for As, Cr, Cu, Hg, Pb, and V. Land use-dependent predictions of spatial patterns split up Europe into investigation areas revealing potentially high (= above-average) or low (= below-average) correlation coefficients. CONCLUSIONS: LDA is an eligible method identifying and ranking boundary conditions of correlations between atmospheric deposition and respective concentrations of heavy metals in moss and related mapping considering the influence of the land use around moss sampling sites.

Anthropogenic and geogenic mass input of trace elements to moss and natural surface soil in Norway.

Data sets for concentrations of up to 22 elements including Pb, Cd, Ag, As, and Hg and several rare earth elements (REEs) in moss and surface soil from all over mainland Norway are analyzed by positive matrix factorization (PMF) and principal component analysis (PCA) with centered log-ratio transformation. Moss and soil samples collected in 2010 and 2005, respectively, show both a distinct long-range atmospheric transport PMF factor including a dominant Pb loading along with smaller loadings of Mo, Cd, Sb, and As, and a geogenic factor dominated by Ce, La, and Y. Other PMF factors for moss and soil are mainly anthropogenic except for two soil factors, a Cr, Co, Ce dominated factor, and an Eu factor. The source area of Eu is mainly inland consistent with its divalent oxidation state. A significant advantage of PMF factors is that their loadings are scaled according to their relative factor contributions. The PMF air pollution factor F3 in moss with average contribution of 7.11µg/g produces an air pollution input of 5.0µg/g which compares well with literature values for the total Pb concentration in moss for 2005 in southern Norway. PCA has the advantage that it can separate factors with very low element concentrations. To support sources of elements identified by PCA it is recommended to include calculation of factor scores to identify significant source areas.

Origin and spatial distribution of metals in moss samples in Albania: A hotspot of heavy metal contamination in Europe.

This study presents the spatial distribution of 37 elements in 48 moss samples collected over the whole territory of Albania and provides information on sources and factors controlling the concentrations of elements in the moss. High variations of trace metals indicate that the concentrations of elements are affected by different factors. Relations between the elements in moss, geochemical interpretation of the data, and secondary effects such as redox conditions generated from local soil and/or long distance atmospheric transport of the pollutants are discussed. Zr normalized data, and the ratios of different elements are calculated to assess the origin of elements present in the current moss samples with respect to different geogenic and anthropogenic inputs. Factor analysis (FA) is used to identify the most probable sources of the elements. Four dominant factors are identified, i.e. natural contamination; dust emission from local mining operations; atmospheric transport of contaminants from local and long distance sources; and contributions from air borne marine salts. Mineral particle dust from local emission sources is classified as the most important factor affecting the atmospheric deposition of elements accumulated in the current moss samples. The open slag dumps of mining operation in Albania is probably the main factor contributing to high contents of Cr, Ni, Fe, Ti and Al in the moss. Enrichment factors (EF) were calculated to clarify whether the elements in the present moss samples mainly originate from atmospheric deposition and/or local substrate materials.

Impact of an iron mine and a nickel smelter at the Norwegian/Russian border close to the Barents Sea on surface soil magnetic susceptibility and content of potentially toxic elements.

An important problem in soil magnetometry is unraveling the soil contamination signal in areas with multiple emitters. Here, geophysical and geochemical measurements were performed at four sites on a north - south transect along the Pasvik River in the Barents Region (northern Norway). These sites are influenced by depositions from the Bjørnevatn iron mine and a Ni-Cu smelter in Nikel, Russia. To relate the degree and type of pollution from these sources to the corresponding magnetic signal, the topsoil concentrations of 12 Potentially Toxic Elements (PTEs) (As, Cd, Co, Cr, Cu, Fe, Mo, Ni, Pb, Se, Ti, Zn), were determined, magnetic hysteresis parameters and thermomagnetic properties were measured. In situ magnetic low-field susceptibility decreases from north to south with increasing distance from the iron mine. Relatively large magnetic multidomain grains of magnetite and/or titanomagnetite are responsible for the strong magnetic signal from the topsoil close to Bjørnevatn. These particles are related to increased enrichment factors of As, Mo and Cu, yielding high positive correlation coefficients with susceptibility values. At a site furthest away from the iron mine and located 7 km from the Ni-Cu smelter magnetic susceptibility values are much lower but significant positive correlations on the level of p < .1 with 8 PTEs (Ni, Cu, Co, Se, As, Zn, Cd, Cr) have been observed. The magnetic signal in this area is due to fine-grained primary sulphides and secondary fine-grained magnetite and/or maghemite.

Integration of soil magnetometry and geochemistry for assessment of human health risk from metallurgical slag dumps.

The main objective of the study was an assessment of the pollution level of agricultural land located close to dumps of industrial waste remaining after former Zn and Pb ore processing in Poland. The integrated geophysical-geochemical methods were applied for assessment of soil quality with respect to trace element pollution. Additionally, human health risk induced by the contaminated arable soil and dusting slag heap was estimated. The investigations pointed out that soils in the vicinity of the metallurgical slag dump in Piekary were heavily polluted. Spatial distribution of magnetic susceptibility corresponding well with distribution of the content of potentially toxic elements indicated the local "pollution hotspots." Proper geophysical and geochemical data interpretation supported by statistical factor analysis enabled identification of three different sources of pollution including metallurgical slug dump as a main source, but also traffic pollution influencing the area located along the busy road and relatively strong influence of the geochemical background. Computed health hazard index revealed no adverse health effect to the farmers cultivating arable soil, but in the direct vicinity of dusting, slag dump health risk occurred, caused mostly by very toxic elements as As and Tl. In the future, investigation should be focused on contribution of different sources to the heavy metal pollution in soil-crop system in this area. It should be highlighted that a site-specific approach should be taken in order to redevelop this kind of area in order to reduce ecological and human health threat. The study proved the integrated two-stage geophysical-geochemical method to be a feasible, reliable, and cost-effective tool for identification of the extent of soil pollution and areas at risk.

The presence of mercury and other trace metals in surface soils in the Norwegian Arctic.

Svalbard is an important study area for investigating the long-range transport of mercury (Hg) and other trace elements to the Arctic. Few studies have focused on their concentrations in Arctic soils. With ongoing climate change leading to thawing permafrost ground the soil compartment is of increasing importance in the Arctic. In this study, elemental composition and soil organic matter (SOM) content of surface and mineral soils in Svalbard are presented. The aim is to provide new data on soils in the Arctic and to gain more knowledge about the role of the soil in the biogeochemical cycle of mercury (Hg). Concentrations are reported for Al, As, Cd, Cr, Cu, Fe, Hg, Mn, Ni, Pb, S and Zn. Samples were taken in Adventdalen and in the area near Ny-Ålesund. We obtained a mean Hg concentration of 0.111 ± 0.036 µg/g in surface soils (range 0.041-0.254 µg/g). Hg levels in mineral soils (mean: 0.025 ± 0.013 µg/g; range: 0.004-0.060 µg/g) were substantially lower than in the corresponding surface soils. Hg strongly accumulates in the surface soil layer (upper 3 cm) and is associated with SOM (surface soil: 59 ± 14%). Hg concentrations in the surface soil were slightly lower than those in the humus layer in mainland Norway and were comparable to levels in soils elsewhere in the Arctic. An inverse association of Hg was found with elements attributed to the mineral soil, indicating that Hg is predominantly derived from atmospheric deposition.

Mass-loss rates from decomposition of plant residues in spruce forests near the northern tree line subject to strong air pollution.

Mass-loss rates during the early phase of decomposition of plant residues were studied for a period of 3 years in Norway spruce forests subjected to air pollution by Cu-Ni smelters on the Kola Peninsula, northwest Russia. Litterbags were deployed in two main patches of forests at the northern tree line, between and below the crowns of spruce trees older than 100 years. The study results demonstrated the dependence of the decomposition rates on the initial concentrations of nutrients and the C/N and lignin/N ratios in plant residues. Lower rates of mass loss in forests subject to air pollution may be related to low quality of plant residues, i.e. high concentrations of heavy metals, low concentrations of nutrients, and high lignin/N and C/N ratios. The increased losses of Ca, Mg, K, and Mn from plant residues in these forests compared to the reference were, probably, related to leaching of their compounds from the residues. The relatively high rates of heavy metal accumulation in the residues were most likely related to uptake of pollutants from the atmosphere, as well as to the lower mass-loss rates. The present study results demonstrate that the forest patchiness should be taken into account in assessment and predictions of decomposition rates in Norway spruce forests. Mass-loss rates of plant residues below the crowns of old spruce trees were significantly lower than those in the patches between the crowns. This was explained by the high C/N and lignin/N ratios in the residues of evergreens which contribute significantly to litterfall below the crowns and by lower soil temperature during winter and spring below the crowns. In addition, a lower amount of precipitation reaching the forest floor below the dense, long crowns of old Norway spruce trees may result in considerably lower washing out of the organic compounds from the residues. Lower mass-loss rates below the crowns of old spruce trees may be part of the evidence that the old-growth spruce forests can continue to accumulate carbon in soil.

Trace elements in native and transplanted Fontinalis antipyretica and Platyhypnidium riparioides from rivers polluted by uranium mining.

The past uranium/polymetallic mining activities in the Sudety (SW Poland) left abandoned mines, pits, and dumps of waste rocks with trace elements and radionuclides which may erode or leach out and create a potential risk for the aquatic ecosystem, among others. In the present work four rivers affected by effluents from such mines were selected to evaluate the application of aquatic mosses for the bioindication of 56 elements. Naturally growing F. antipyretica and P. riparioides were compared with transplanted samples of the same species. The results demonstrate serious pollution of the examined rivers, especially with As, Ba, Fe, Mn, Pb, Ti, U and Zn, reaching extremely high concentrations in native moss samples. In the most polluted rivers native F. antipyretica and P. riparioides samples showed significantly higher concentrations of As, Ba, Cu, Fe, La, Nd, Ni, Pb, U and Zn than corresponding transplanted samples, whereas at less polluted sites a reverse situation was sometimes observed. Transplanted moss moved from clean to extremely polluted rivers probably protects itself against the accumulation of toxic elements by reducing their uptake. Selection of native or transplanted F. antipyretica and P. riparioides depended on the pollution load.

Dust is the dominant source of "heavy metals" to peat moss (Sphagnum fuscum) in the bogs of the Athabasca Bituminous Sands region of northern Alberta.

Sphagnum fuscum was collected from twenty-five ombrotrophic (rain-fed) peat bogs surrounding open pit mines and upgrading facilities of Athabasca Bituminous Sands (ABS) in northern Alberta (AB) in order to assess the extent of atmospheric contamination by trace elements. As a control, this moss species was also collected at a bog near Utikuma (UTK) in an undeveloped part of AB and 264km SW of the ABS region. For comparison, this moss was also collected in central AB, in the vicinity of the City of Edmonton which is approximately 500km to the south of the ABS region, from the Wagner Wetland which is 22km W of the City, from Seba Beach (ca. 90km W) and from Elk Island National Park (ca. 45km E). All of the moss samples were digested and trace elements concentrations determined using ICP-SMS at a commercial laboratory, with selected samples also analyzed using instrumental neutron activation analysis at the University of Alberta. The mosses from the ABS region yielded lower concentrations of Ag, As, Bi, Cd, Cu, Pb, Sb, Tl, and Zn compared to the moss from the Edmonton area. Concentrations of Ni and Mo in the mosses were comparable in these two regions, but V was more abundant in the ABS samples. Compared with the surface vegetation of eight peat cores collected in recent years from British Columbia, Ontario, Quebec and New Brunswick, the mean concentrations of Ag, As, Bi, Cd, Cu, Mo, Ni, Pb, Sb, Tl and Zn in the mosses from the ABS region are generally much lower. In fact, the concentrations of these trace elements in the samples from the ABS region are comparable to the corresponding values in forest moss from remote regions of central and northern Norway. Lithophile element concentrations (Ba, Be, Ga, Ge, Li, Sc, Th, Ti, Zr) explain most of the variation in trace metal concentrations in the moss samples. The mean concentrations of Th and Zr are greatest in the moss samples from the ABS region, reflecting dust inputs to the bogs from open pit mines, aggregate quarries, and gravel roads. Linear regressions of V, Ni, and Mo (elements enriched in bitumen) versus Sc (a conservative, lithophile element) show excellent correlations in the mosses from the ABS region, but this is true also of Ag, Pb, Sb and Tl: thus, most of the variation in the trace metal concentrations can be explained simply by the abundance of dust particles on the plants of this region. Unlike the moss samples from the ABS region and from UTK where Pb/Sc ratios resemble those of crustal rocks, the moss samples from the other regions studied yielded much greater Pb/Sc ratios implying significant anthropogenic Pb contributions at these other sites.

Spatially valid data of atmospheric deposition of heavy metals and nitrogen derived by moss surveys for pollution risk assessments of ecosystems.

For analysing element input into ecosystems and associated risks due to atmospheric deposition, element concentrations in moss provide complementary and time-integrated data at high spatial resolution every 5 years since 1990. The paper reviews (1) minimum sample sizes needed for reliable, statistical estimation of mean values at four different spatial scales (European and national level as well as landscape-specific level covering Europe and single countries); (2) trends of heavy metal (HM) and nitrogen (N) concentrations in moss in Europe (1990-2010); (3) correlations between concentrations of HM in moss and soil specimens collected across Norway (1990-2010); and (4) canopy drip-induced site-specific variation of N concentration in moss sampled in seven European countries (1990-2013). While the minimum sample sizes on the European and national level were achieved without exception, for some ecological land classes and elements, the coverage with sampling sites should be improved. The decline in emission and subsequent atmospheric deposition of HM across Europe has resulted in decreasing HM concentrations in moss between 1990 and 2010. In contrast, hardly any changes were observed for N in moss between 2005, when N was included into the survey for the first time, and 2010. In Norway, both, the moss and the soil survey data sets, were correlated, indicating a decrease of HM concentrations in moss and soil. At the site level, the average N deposition inside of forests was almost three times higher than the average N deposition outside of forests.

Background levels of some major, trace, and rare earth elements in indigenous plant species growing in Norway and the influence of soil acidification, soil parent material, and seasonal variation on these levels.

Baseline levels of 43 elements, including major, trace, and rare earth elements (REEs) in several native plant species growing in boreal and alpine areas, are presented. Focus is placed on species metal levels at different soil conditions, temporal variations in plant tissue metal concentrations, and interspecies variation in metal concentrations. Vegetation samples were collected at Sogndal, a pristine site in western Norway, and at Risdalsheia, an acidified site in southernmost Norway. Metal concentrations in the different species sampled in western Norway are compared with relevant literature data from Norway, Finland, and northwest Russia, assumed to represent natural conditions. Except for aluminium (Al) and macronutrients, the levels of metals were generally lower in western Norway than in southern Norway and may be considered close to natural background levels. In southern Norway, the levels of cadmium (Cd) and lead (Pb) in particular appear to be affected by air pollution, either by direct atmospheric supply or through soil acidification. Levels of some elements show considerable variability between as well as within plant species. Calcium (Ca), magnesium (Mg), and potassium (K) are higher in most species at Sogndal compared to Risdalsheia, despite increased extractable concentrations in surface soil in the south, probably attributed to different buffer mechanisms in surface soil. Antagonism on plant uptake is suggested between Ca, Mg, and K on one hand and Al on the other. Tolerance among calcifuges to acid conditions and a particular ability to detoxify or avoid uptake of Al ions are noticeable for Vaccinium vitis-idaea.

Essential and non-essential elements in natural vegetation in southern Norway: contribution from different sources.

Concentrations of essential and non-essential elements in five widespread species of natural boreal vegetation were studied with respect to seasonal variation and contribution from different sources. The plant species included in the study were Betula pubescens, Sorbus aucuparia, Vaccinium myrtillus, Vaccinium uliginosum, Calluna vulgaris and Deschampsia flexuosa. Concentrations of elements essential to plants remained essentially constant or decreased slightly throughout the growing season. Concentrations of most non-essential elements increased or tended to increase on a dry mass basis from June to July as well as from July to September. The increasing trend for these elements was observed for all species except C. vulgaris. Principal component analysis (PCA) of the material indicated a common source for many of the non-essential elements; Sc, Ti, V, Ga, As, Y, Sb, lanthanides, Pb, Bi, and U, i.e. both elements presumably of geogenic origin and elements associated with trans-boundary air pollution. Uptake by plant roots appeared to be the main source of nutrient elements as well as some non-essential elements.

Endosulfan, pentachlorobenzene and short-chain chlorinated paraffins in background soils from Western Europe.

Soils are major reservoirs for many persistent organic pollutants (POPs). In this study, "newly" regulated POPs i.e. Σendosulfans (α-endosulfan, ß-endosulfan, endosulfan sulfate), pentachlorobenzene (PeCB), and short-chain chlorinated paraffins (SCCPs) were determined in background samples from woodland (WL) and grassland (GL) surface soil, collected along an existing latitudinal UK-Norway transect. Statistical analysis, complemented with plots showing the predicted equilibrium distribution and mobility potential, was then explored to discuss factors controlling their spatial distribution. SCCPs were detected with the highest average concentrations (35 ± 100 ng/g soil organic matter (SOM)), followed by Σendosulfans (3 ± 3 ng/g SOM) and PeCB (1 ± 1 ng/g SOM). PeCB and Σendosulfans share many similarities in their distribution in these background soils as well as with several legacy POPs. A steep decline in concentrations of SCCPs with increasing latitude indicates that their occurrence is dictated by proximity to source regions, while concentrations of Σendosulfans peaked in regions experiencing elevated precipitation rates.

Correlating concentrations of heavy metals in atmospheric deposition with respective accumulation in moss and natural surface soil for ecological land classes in Norway between 1990 and 2010.

This study investigated whether statistical correlation of modeled atmospheric heavy metal deposition and respective accumulation in moss and natural surface soil varies across natural landscapes in Norway. Target metals were cadmium, lead, and mercury, and analyses were run between 1990 and 2010 on a 5-year interval. The landscape information was derived from the Ecological Land Classification of Europe. Correlations between concentration and respective deposition data were computed for each land class. The strongest correlations between heavy metal concentrations in atmospheric deposition and corresponding levels in moss and natural surface soil were observed for lead. Correlations for mercury were weaker compared to those calculated for cadmium and lead, indicating that atmospheric transport of mercury occurs at a larger spatial scale, while accumulation additionally seems to be influenced by factors operating on smaller scales. The correlation between concentrations in atmospheric deposition and moss is landscape-specific and metal-specific. The same holds true for the relations between heavy metal concentration in modeled atmospheric deposition and natural surface soil. The results of this investigation are in line with similar calculations from across Europe. They further confirm previous studies indicating that for Norway atmospheric transport is a main source of lead and cadmium accumulation in moss as well as in natural surface soil.

Leaching of polycyclic aromatic hydrocarbons from oil shale processing waste deposit: a long-term field study.

The leaching behavior of selected polycyclic aromatic hydrocarbons (PAHs) from an oil shale processing waste deposit was monitored during 2005-2009. Samples were collected from the deposit using a special device for leachate sampling at field conditions without disturbance of the upper layers. Contents of 16 priority PAHs in leachate samples collected from aged and fresh parts of the deposit were determined by GC-MS. The sum of the detected PAHs in leachates varied significantly throughout the study period: 19-315 µg/l from aged spent shale, and 36-151 µg/l from fresh spent shale. Among the studied PAHs the low-molecular weight compounds phenanthrene, naphthalene, acenaphthylene, and anthracene predominated. Among the high-molecular weight PAHs benzo[a]anthracene and pyrene leached in the highest concentrations. A spent shale deposit is a source of PAHs that could infiltrate into the surrounding environment for a long period of time.

Geographical trends in 137Cs fallout from the Chernobyl accident and leaching from natural surface soil in Norway.

In order to follow the turnover of (137)Cs in natural soils and estimate future trends in exposure of livestock, samples of natural surface soils were collected at 0-3 cm depth at 464 sites in 1995 and 463 sites in 2005 covering the country. In both cases the geographical pattern observed was similar to the original distribution from 1986, but the decline of (137)Cs activity in the surface soil was not the same everywhere. In 1995 the (137)Cs reduction since 1986 was found to be considerably greater in coastal areas than farther inland. The main reason for this appears to be the much greater deposition of marine cations such as Mg(2+) and Na(+) in the coastal areas, replacing Cs ions fixed on soil particle surfaces. This cation exchange appeared to be particularly strong near the southern coast where deposition of NH4(+) from transboundary air pollution is evident in addition to the marine cations. During 1995-2005 the (137)Cs decline in the surface soil was more uniform over the country than in the preceding 10-year period but still significantly higher in coastal areas than inland. Differences in precipitation chemistry may have influenced the uptake of (137)Cs in terrestrial food chains.