Quarter century of mercury litterfall at a coniferous forest responding to climate change, Central Europe.

This work evaluated the 25-year-long trends (1994-2018) in mercury (Hg) concentrations and fluxes in spruce litterfall at a forest research plot Nacetín (NAC) recovering from acidic deposition in the Ore Mountains, Czech Republic. The mean litterfall Hg deposition averaged 51 ± 18 µg m-2 year-1, which has been the highest litterfall Hg deposition reported up to date on the European continent. In contrast, the wet deposition (2017-2019) was an order of magnitude lower averaging at 2.5 ± 1.5 µg m-2 year-1. All the spruce litterfall components bark, twigs, needles, cones, and a mixture of unidentified fragments had elevated mean Hg concentrations relative to background sites averaging 256 ± 77, 234 ± 62, 119 ± 23, 95 ± 14, and 44 ± 15 µg kg-1, respectively. Elevated litterfall Hg deposition and concentrations were attributed to the nearby local Hg emission source-coal-fired power plants. Temporally, the decrease of Czech Hg emissions since the 1990s was reflected by the decreasing trend of Hg concentrations in litterfall bark, cones, and twigs, while in needles and other material, Hg increased but insignificantly. Total litterfall ratios of Hg/C, Hg/N, and Hg/S were lower than those in soil O horizons averaging at 0.23 ± 0.04, 9.5 ± 2.0, and 170 ± 37 µg g-1, respectively. Since the beginning of monitoring, total litterfall Hg/C exhibited no trend, Hg/N decreased, and Hg/S increased. The litterfall biomass deposition averaging at 469 ± 176 g m-2 year-1 increased through time resulting in an increased Hg litterfall deposition at NAC by 1.1 µg m-2 year-1 despite the decreases in Czech Hg emissions. Peaks of annual litterfall Hg deposition up to 96 µg m-2 year-1 at NAC during the 25 years of monitoring resulted from weather extremes such as rime-snow accumulation, wind gusts, droughts, and insect infestation, which all significantly affected the annual biomass deposition. Based on our observations, further increases in biomass and litterfall Hg deposition rates can be expected due to the onset of bark beetle infestation and the increasing number of droughts caused by climate change.

Response of spring yield dynamics to climate change across altitude gradient and varied hydrogeological conditions.

Springs offer insights into groundwater dynamics. Long-term monitoring of spring yields can reflect the response of groundwater storage to climate change. We analyzed the yield trends of 136 springs across 18 hydrogeological regions in Czechia from 1971 to 2020. The trend-free pre-whitening Mann-Kendall test and linear mixed-effects models were used to assess environmental impacts on spring yields. Overall, 71 % of the springs showed no long-term trends, 28 % exhibited decreasing trends, and 1.5 % showed increasing trends in annual spring yields. Altitude has been demonstrated as a contributing factor influencing spring responses to climate change. Lowland springs (<300 m a.s.l.) exhibited the highest proportion of decreasing annual trends (41 %), while uplands (300-600 m a.s.l.) and highlands (>600 m a.s.l.) showed declines in 26 % and 25 % of springs, respectively. Moreover, highlands recorded a 7 % yield increase, indicating a complex interplay between altitude and spring response to climatic factors. A strong positive correlation was found between precipitation and yields (p < 0.01), whereas temperature increases negatively affected spring yields (p < 0.01). The interaction between temperature changes and region transmissivity highlighted the vulnerability of springs in low-transmissivity regions, predominantly those in crystalline and flysch bedrock areas, to climatic shifts. Generally, these regions have lower spring yields compared to the high-transmissivity areas of the Cretaceous basins. Although these lower-yield regions are not used as a primary water source for large areas, unlike regions with high-transmissivity bedrock, they provide water resources for local supply. Analysis of annual spring maxima frequencies revealed a shift in the culmination of maxima occurrences from April to March, with a significant decrease in April (p < 0.05) and May (p < 0.1) and an increase in March (p < 0.05), suggesting a change in spring yield seasonality. The 2015-2020 drought significantly accelerated declining spring yield trends across hydrogeological regions.

Carbon and nutrient pools and fluxes in unmanaged mountain Norway spruce forests, and losses after natural tree dieback.

Forest areas infected by insects are increasing in Europe and North America due to accelerating climate change. A 2000-2020 mass budget study on major elements (C, N, P, Ca, Mg, K) in the atmosphere-plant-soil-water systems of two unmanaged catchments enabled us to evaluate changes in pools and fluxes related to tree dieback and long-term accumulation/losses during the post-glacial period. A bark-beetle outbreak killed >75 % of all trees in a mature mountain spruce forest in one catchment and all dead biomass was left on site. A similar forest in a nearby catchment was only marginally affected. We observed that: (1) the long-term (millennial) C and N accumulation in soils averaged 10-22 and 0.5-1.1 kg ha-1 yr-1, respectively, while losses of Ca, Mg, and K from soils ranged from 0.1 to 2.6 kg ha-1 yr-1. (2) Only <0.8 % and <1.5 % of the respective total C and N fluxes entering the soil annually from vegetation were permanently stored in soils. (3) The post-disturbance decomposition of dead tree biomass reduced vegetation element pools from 27 % (C) to 73 % (P) between 2004 and 2019. (4) Tree dieback decreased net atmospheric element inputs to the impacted catchment, and increased the leaching of all elements and gaseous losses of C (∼2.3 t ha-1 yr-1) and N (∼14 kg ha-1 yr-1). The disturbed catchment became a net C source, but ∼50 % of the N released from dead biomass accumulated in soils. (5) Despite the severe forest disturbance, the dissolved losses of Ca and Mg represented 52-58 % of their leaching from intact stands during the peaking atmospheric acidification from 1970 to 1990. (6) Disturbance-related net leaching of P, Ca, Mg, and K were 4, 69, 16, and 114 kg ha-1, respectively, which represented 7-38 % of the losses potentially related to sanitary logging and subsequent removal of the aboveground tree biomass.

Ammonia oxidation and nitrate reduction marker genes are key indicators of nitrogen losses in temperate forest catchments.

Chronic nitrogen inputs can alleviate N limitation and potentially impose N losses in forests, indicated by soil enrichment in 15 N over 14 N. However, the complexity of the nitrogen cycle hinders accurate quantification of N fluxes. Simultaneously, soil ecologists are striving to find meaningful indicators to characterise the "openness" of the nitrogen cycle. We integrate soil δ15 N with constrained ecosystem N losses and the functional gene potential of the soil microbiome in 14 temperate forest catchments. We show that N losses are associated with soil δ15 N and that δ15 N scales with the abundance of soil bacteria. The abundance of the archaeal amoA gene, representing the first step in nitrification (ammonia oxidation to nitrite), followed by the abundance of narG and napA genes, associated with the first step in denitrification (nitrate reduction to nitrite), explains most of the variability in soil δ15 N. These genes are more informative than the denitrification genes nirS and nirK, which are directly linked to N2 O production. Nitrite formation thus appears to be the critical step associated with N losses. Furthermore, we show that the genetic potential for ammonia oxidation and nitrate reduction is representative of forest soil 15 N enrichment and thus indicative of ecosystem N losses.

Forest growth responds more to air pollution than soil acidification.

The forests of central Europe have undergone remarkable transitions in the past 40 years as air quality has improved dramatically. Retrospective analysis of Norway spruce (Picea abies) tree rings in the Czech Republic shows that air pollution (e.g. SO2 concentrations, high acidic deposition to the forest canopy) plays a dominant role in driving forest health. Extensive soil acidification occurred in the highly polluted "Black Triangle" in Central Europe, and upper mineral soils are still acidified. In contrast, acidic atmospheric deposition declined by 80% and atmospheric SO2 concentration by 90% between the late 1980s and 2010s. In this study we oserved that annual tree ring width (TRW) declined in the 1970s and subsequently recovered in the 1990s, tracking SO2 concentrations closely. Furthermore, recovery of TRW was similar in unlimed and limed stands. Despite large increases in soil base saturation, as well as soil pH, as a result of repeated liming starting in 1981, TRW growth was similar in limed and unlimed plots. TRW recovery was interrupted in 1996 when highly acidic rime (originating from more pronounced decline of alkaline dust than SO2 from local power plants) injured the spruce canopy, but recovered soon to the pre-episode growth. Across the long-term site history, changes in soil chemistry (pH, base saturation, Bc/Al soil solution ratio) cannot explain observed changes in TRW at the two study sites where we tracked soil chemistry. Instead, statistically significant recovery in TRW is linked to the trajectory of annual SO2 concentrations or sulfur deposition at all three stands.

Increasing water-use efficiency mediates effects of atmospheric carbon, sulfur, and nitrogen on growth variability of central European conifers.

Climate controls forest biomass production through direct effects on cambial activity and indirectly through interactions with CO2, air pollution, and nutrient availability. The atmospheric concentration of CO2, sulfur and nitrogen deposition can also exert a significant indirect control on wood formation since these factors influence the stomatal regulation of transpiration and carbon uptake, that is, intrinsic water use efficiency (iWUE). Here we provide 120-year long tree-ring time series of iWUE, stem growth, climatic and combined sulfur and nitrogen (SN) deposition trends for two common tree species, Pinus sylvestris (PISY) and Picea abies (PCAB), at their lower and upper distribution margins in Central Europe. The main goals were to explain iWUE trends using theoretical scenarios including climatic and SN deposition data, and to assess the contribution of climate and iWUE to the observed growth trends. Our results showed that after a notable increase in iWUE between the 1950s and 1980s, this positive trend subsequently slowed down. The substantial rise of iWUE since the 1950s resulted from a combination of an accelerated increase in atmospheric CO2 concentrations (Ca) and a stable level of leaf intercellular CO2 (Ci). The offset of observed iWUE values above the trajectory of a constant Ci/Ca scenario was explained by trends in SN deposition (all sites) together with the variation of drought conditions (low-elevation sites only). Increasing iWUE over the 20th and 21st centuries improved tree growth at low-elevation drought-sensitive sites. In contrast, at high-elevation PCAB sites, growth was mainly stimulated by recent warming. We propose that SN pollution should be considered in order to explain the steep increase in iWUE of conifers in the 20th century throughout Central Europe and other regions with a significant SN deposition history.

Changes in forest nitrogen cycling across deposition gradient revealed by δ15N in tree rings.

Tree rings provide valuable insight into past environmental changes. This study aimed to evaluate perturbations in tree ring width (TRW) and δ15N alongside soil acidity and nutrient availability gradients caused by the contrasting legacy of air pollution (nitrogen [N] and sulphur [S] deposition) and tree species (European beech, Silver fir and Norway spruce). We found consistent declines of tree ring δ15N, which were temporarily unrelated to the changes in the TRW. The rate of δ15N change in tree rings was related to the contemporary foliar carbon (C) to phosphorus (P) ratio. This observation suggested that the long-term accumulation of 15N depleted N in tree rings, likely mediated by retained N from deposition, was restricted primarily to stands with currently higher P availability. The shifts observed in tree-ring δ15N and TRW suggest that acidic air pollution rather than changes in stand productivity determined alteration of N and C cycles. Stable N isotopes in tree rings provided helpful information on the trajectory of the N cycle over the last century with direct consequences for a better understanding of future interactions among N, P and C cycles in terrestrial ecosystems.

Catchment Runoff in Industrial Areas Exports Legacy Pollutant Zinc from the Topsoil Rather than Geogenic Zn.

In highly industrialized, densely populated parts of Central Europe, mobilization of legacy Zn pollution from forest ecosystems may negatively affect the quality of water resources. To test this hypothesis, we determined the 66Zn/64Zn isotope ratios of 15 Zn reservoirs and fluxes in an acidified, spruce die-back affected mountain-slope catchment in northern Czech Republic. The δ66Zn values of precipitation, organic horizon, and runoff were statistically indistinguishable. In contrast, δ66Zn values of bedrock orthogneiss and mineral soil were significantly different from δ66Zn values of runoff. The magnitude of within-site Zn isotope fractionations appeared to be relatively small. Despite the large potential source of Zn in bedrock, runoff exported mostly young pollutant Zn that had been temporarily stored in the organic horizon. This conclusion was corroborated by comparing Zn input-output mass balances in the polluted northern catchment and in a relatively unpolluted catchment situated 250 km to the south. Seven-times higher Zn export via runoff at the northern site was controlled by a combination of 10-times higher atmospheric Zn input and five-times higher DOC leaching, compared to the southern site. In industrial areas, atmospherically deposited Zn is leached from headwater catchments in a direct analogy to leaching of highly toxic pollutant Pb.

Bacteria but not fungi respond to soil acidification rapidly and consistently in both a spruce and beech forest.

Anthropogenically enhanced atmospheric sulphur (S) and nitrogen (N) deposition has acidified and eutrophied forest ecosystems worldwide. However, both S and N mechanisms have an impact on microbial communities and the consequences for microbially driven soil functioning differ. We conducted a two-forest stand (Norway spruce and European beech) field experiment involving acidification (sulphuric acid addition) and N (ammonium nitrate) loading and their combination. For 4 years, we monitored separate responses of soil microbial communities to the treatments and investigated the relationship to changes in the activity of extracellular enzymes. We observed that acidification selected for acidotolerant and oligotrophic taxa of Acidobacteria and Actinobacteria decreased bacterial community richness and diversity in both stands in parallel, disregarding their original dissimilarities in soil chemistry and composition of microbial communities. The shifts in bacterial community influenced the stoichiometry and magnitude of enzymatic activity. The bacterial response to experimental N addition was much weaker, likely due to historically enhanced N availability. Fungi were not influenced by any treatment during 4-year manipulation. We suggest that in the onset of acidification when fungi remain irresponsive, bacterial reaction might govern the changes in soil enzymatic activity.

Disruptions and re-establishment of the calcium-bicarbonate equilibrium in freshwaters.

During recent decades, increasing anthropogenic activities have affected natural ionic composition, including the strongest and most common relationship between ionic concentrations in the majority of natural global freshwaters, i.e., the Ca2+-ANC (acid neutralizing capacity) equilibrium. Using long-term monitoring data and MAGIC modelling, we evaluated effects of major present environmental stressors (synthetic fertilizers, liming, acidic deposition, forest disturbances, and climate change) on the Ca2+-ANC equilibrium. We evaluated the effects for three different types of terrestrial ecosystems, a circumneutral lowland agricultural catchment, two acid sensitive mountain forest catchments differing in forest health, and one acid sensitive alpine catchment. All catchments are in a region with the world-largest changes in fertilizing rates and acidic deposition in the 20th century, with increasing impacts until the late 1980s, and their subsequent abrupt, dramatic decreases. These strong changes resulted in a substantial disruption, followed by continuing re-establishment of the Ca2+-ANC relationship in all study waters. The shape of the disruption and the following re-establishment of its new value were dependent on the intensity, duration, and combination of stressors, as well as on catchment characteristics (bedrock composition, soil amount and composition, vegetation status, and hydrology). We conclude that a new equilibrium may deviate from its natural value due to the (1) legacy of fertilizing, acidic deposition and liming, affecting the soil Ca2+ pools, (2) forest disturbances and management practices, and (3) climate change.

Comparison of the impacts of acid and nitrogen additions on carbon fluxes in European conifer and broadleaf forests.

Increased reactive nitrogen (N) loadings to terrestrial ecosystems are believed to have positive effects on ecosystem carbon (C) sequestration. Global "hot spots" of N deposition are often associated with currently or formerly high deposition of sulphur (S); C fluxes in these regions might therefore not be responding solely to N loading, and could be undergoing transient change as S inputs change. In a four-year, two-forest stand (mature Norway spruce and European beech) replicated field experiment involving acidity manipulation (sulphuric acid addition), N addition (NH4NO3) and combined treatments, we tested the extent to which altered soil solution acidity or/and soil N availability affected the concentration of soil dissolved organic carbon (DOC), soil respiration (Rs), microbial community characteristics (respiration, biomass, fungi and bacteria abundances) and enzyme activity. We demonstrated a large and consistent suppression of soil water DOC concentration driven by chemical changes associated with increased hydrogen ion concentrations under acid treatments, independent of forest type. Soil respiration was suppressed by sulphuric acid addition in the spruce forest, accompanied by reduced microbial biomass, increased fungal:bacterial ratios and increased C to N enzyme ratios. We did not observe equivalent effects of sulphuric acid treatments on Rs in the beech forest, where microbial activity appeared to be more tightly linked to N acquisition. The only changes in C cycling following N addition were increased C to N enzyme ratios, with no impact on C fluxes (either Rs or DOC). We conclude that C accumulation previously attributed solely to N deposition could be partly attributable to their simultaneous acidification.

Author Correction: Microbial communities with distinct denitrification potential in spruce and beech soils differing in nitrate leaching.

A correction to this article has been published and is linked from the HTML and PDF versions of this paper. The error has not been fixed in the paper.

Microbial communities with distinct denitrification potential in spruce and beech soils differing in nitrate leaching.

Nitrogen leaching owing to elevated acid deposition remains the main ecosystem threat worldwide. We aimed to contribute to the understanding of the highly variable nitrate losses observed in Europe after acid deposition retreat. Our study proceeded in adjacent beech and spruce forests undergoing acidification recovery and differing in nitrate leaching. We reconstructed soil microbial functional characteristics connected with nitrogen and carbon cycling based on community composition. Our results showed that in the more acidic spruce soil with high carbon content, where Acidobacteria and Actinobacteria were abundant (Proteo:Acido = 1.3), the potential for nitrate reduction and loss via denitrification was high (denitrification: dissimilative nitrogen reduction to ammonium (DNRA) = 3). In the less acidic beech stand with low carbon content, but high nitrogen availability, Proteobacteria were more abundant (Proteo:Acido = 1.6). Proportionally less nitrate could be denitrified there (denitrification:DNRA = 1), possibly increasing its availability. Among 10 potential keystone species, microbes capable of DNRA were identified in the beech soil while instead denitrifiers dominated in the spruce soil. In spite of the former acid deposition impact, distinct microbial functional guilds developed under different vegetational dominance, resulting in different N immobilization potentials, possibly influencing the ecosystem's nitrogen retention ability.

Environmental factors exert strong control over the climate-growth relationships of Picea abies in Central Europe.

The growth response of trees to changing climate is frequently discussed as increasing temperatures and more severe droughts become major risks for forest ecosystems. However, the ability of trees to cope with the changing climate and the effects of other environmental factors on climate-growth relationships are still poorly understood. There is thus an increasing need to understand the ability of individual trees to cope with changing climate in various environments. To improve the current understanding, a large tree-ring network covering the whole area of the Czech Republic (in 7×7km grids) was utilized to investigate how the climate-growth relationships of Norway spruce are affected by 1) various geographical variables, 2) changing levels of acidic deposition, 3) soil characteristics and 4) age, tree diameter and neighbourhood competition. The period from 1930 to 2013 was divided into four, 21-year long intervals of differing levels of acidic deposition, which peaked in the 1972-1993 period. Our individual-based, spatiotemporal, multivariate analyses revealed that spruce growth was mostly affected by drought and warm summers. Drought plays the most important negative role at lower altitudes, while the positive effect of higher temperature was identified for trees at higher altitudes. Increased levels of acidic deposition, together with geographical variables, were identified as the most important factors affecting climate-growth association. Tree age, tree size and soil characteristics also significantly modulate climate-growth relationships. The importance of all environmental variables on climate-growth relationships was suppressed by acidic deposition during periods when this was at a high level; growth was significantly more enhanced by spring and summer temperatures during these periods. Our results suggest that spruce will undergo significant growth reduction under the predicted climate changes, especially at the lower altitudes which lie outside of its natural range.

Discerning environmental factors affecting current tree growth in Central Europe.

We examined the effect of individual environmental factors on the current spruce tree growth assessed from a repeated country-level statistical landscape (incl. forest) survey in the Czech Republic. An extensive set of variables related to tree size, competition, site characteristics including soil texture, chemistry, N deposition and climate was tested within a random-effect model to explain growth in the conditions of dominantly managed forest ecosystems. The current spruce basal area increment was assessed from two consecutive landscape surveys conducted in 2008/2009 and six years later in 2014/2015. Tree size, age and competition within forest stands were found to be the dominant explanatory variables, whereas the expression of site characteristics, environmental and climatic drives was weaker. The significant site variables affecting growth included soil C/N ratio and soil exchangeable acidity (pH KCl; positive response) reflecting soil chemistry, long-term N-deposition (averaged since 1975) in combination with soil texture (clay content) and Standardized Precipitation Index (SPI), a drought index expressing moisture conditions. Sensitivity of growth to N-deposition was positive, although weak. SPI was positively related to and significant in explaining tree growth when expressed for the growth season. Except SPI, no significant relation of growth was determined to altitude-related variables (temperature, growth season length). We identified the current spruce growth optimum at elevations about 800ma.s.l. or higher in the conditions of the country. This suggests that at lower elevations, limitation by a more pronounced water deficit dominates, whereas direct temperature limitation may concern the less frequent higher elevations. The mixed linear model of spruce tree growth explained 55 and 65% of the variability with fixed and random effects included, respectively, and provided new insights on the current spruce tree growth and factors affecting it within the environmental gradients of the country.

Effect of industrial dust on precipitation chemistry in the Czech Republic (Central Europe) from 1850 to 2013.

Using statistical relationships between the composition of precipitation at eight long-term monitoring stations and emission rates of sulphur (S) and nitrogen (N) compounds, as well as industrial dust in the Czech Republic and Slovakia (Central Europe), we modelled historic pH and concentrations of sulphate (SO4(2-)), nitrate (NO3(-)), ammonium (NH4(+)), chloride (Cl(-)), base cations (BC), and bicarbonate (HCO3(-)) in bulk precipitation from 1850 to 2013. Our model suggests that concentrations of SO4(2-), NO3(-), and HCO3(-) were similar (11-16 µeq l(-1)) in 1850. Cations were dominated by NH4(+) and BC (24-27 µeq l(-1)) and precipitation pH was >5.6. The carbonate buffering system was depleted around 1920 and precipitation further acidified at an exponential rate until the 1980s, when concentrations of SO4(2-), NO3(-), Cl(-), NH4(+) and BC reached maxima of 126, 55, 16, 76, and 57 µeq l(-1), respectively, and pH decreased to 4.2. Dust emissions from industrial sources were an important source of BC. Without their contribution, pH would have decreased to 4.0 in the 1980s, and the carbonate buffering system would have been depleted already in the 1870s. Since the late 1980s, concentrations of strong acid anions and BC have decreased by 46-81% (i.e. more than in Europe on average) due to a 53-93% reduction in regional emissions of S and N compounds and dust from industrial and agricultural sources. The present composition of precipitation is similar to the late 19th century, except for NO3(-) concentrations, which are similar to those during 1926-1950. Precipitation pH now exceeds 5.0, the carbonate buffering system has been re-established, and HCO3(-) has again become (after almost a century) a significant component of precipitation chemistry.

Pollution control enhanced spruce growth in the "Black Triangle" near the Czech-Polish border.

Norway spruce (Picea abies (L.) Karst.) stands in certain areas of Central Europe have experienced substantial dieback since the 1970s. Understanding the reasons for this decline and reexamining the response of forests to acid deposition reduction remains challenging because of a lack of long and well-replicated tree-ring width chronologies. Here, spruce from a subalpine area heavily affected by acid deposition (from both sulfur and nitrogen compounds) is evaluated. Tree-ring width measurements from 98 trees between 1000 and 1350m above sea level (a.s.l.) reflected significant May-July temperature signals. Since the 1970s, acid deposition has reduced the growth-climate relationship. Efficient pollution control together with a warmer but not drier climate most likely caused the increased growth of spruce stands in this region, the so-called "Black Triangle," in the 1990s.

Does stream water chemistry reflect watershed characteristics?

In this study, we investigated the relationships between stream water chemistry and watershed characteristics (topography--mean altitude and slope; climate--mean annual temperature and precipitation; geology--geochemical reactivity; land cover; inhabitation--population density, road density and number of municipalities). We analyzed the concentrations of the major anions (Cl, F, NO3, SO4, SiO2), cations (Ca, Mg, Na, K, Mn, Fe, Al), trace elements (Li, Sr, Cu), ABS245, TDP (total dissolved phosphorus), pH, and conductivity at 3,220 diverse watersheds covering a wide variety of watershed characteristics in the Czech Republic. We used marginal and partial multivariate analyses to reveal the most important variables. The partial analysis showed that only 14% of the variance could be assigned to a specific factor and that 41% of the variance is shared among the factors, which indicated complex interactions between the watershed characteristics.

Long-term changes in aluminum fractions of drainage waters in two forest catchments with contrasting lithology.

Aluminum (Al) chemistry was studied in soils and waters of two catchments covered by spruce (Picea abies) monocultures in the Czech Republic that represent geochemical end-members of terrestrial and aquatic sensitivity to acidic deposition. The acid-sensitive Lysina catchment, underlain by granite, was compared to the acid-resistant Pluhuv Bor catchment on serpentine. Organically-bound Al was the largest pool of reactive soil Al at both sites. Very high median total Al (Alt) concentrations (40 micromol L(-1)) and inorganic monomeric Al (Ali) concentrations (27 micromol L(-1)) were observed in acidic (pH 4.0) stream water at Lysina in the 1990s and these concentrations decreased to 32 micromol L(-1) (Alt) and 13 micromol L(-1) (Ali) in the 2000s. The potentially toxic Ali fraction decreased in response to long-term decreases in acidic deposition, but Ali remained the largest fraction. However, the organic monomeric (Alo) and particulate (Alp) fractions increased in the 2000s at Lysina. In contrast to Lysina, marked increases of Alt concentrations in circum-neutral waters at Pluhuv Bor were observed in the 2000s in comparison with the 1990s. These increases were entirely due to the Alp fraction, which increased more than 3-fold in stream water and up to 8-fold in soil water in the A horizon. Increase of Alp coincided with dissolved organic carbon (DOC) increases. Acidification recovery may have increased the content of colloidal Al though the coagulation of monomeric Al.

Rising trends of dissolved organic matter in drinking-water reservoirs as a result of recovery from acidification in the Ore Mts., Czech Republic.

The concentration of chemical oxygen demand (COD), a common proxy for dissolved organic matter (DOM), was measured at seven drinking-water reservoirs and four streams between 1969 and 2006. Nine of them showed significant DOM increases (median COD change +0.08 mg L(-1) yr(-1)). Several potential drivers of these trends were considered, including air temperature, rainfall, land-use and water sulfate concentration. Temperature and precipitation influenced inter-annual variations, but not long-term trends. The long-term DOM increase was significantly associated with declines of acidic deposition, especially sulfur deposition. Surface water sulfate concentrations decreased from a median of 62 mg L(-1)-27 mg L(-1) since 1980. The magnitude of DOM increase was positively correlated with average DOM concentration (R(2) = 0.79, p < 0.001). Simultaneously, DOM concentration was positively correlated with the proportion of Histosols within the catchments (R(2) = 0.79, p < 0.001). A focus on the direct removal of DOM by water treatment procedures rather than catchment remediation is needed.