Use of the Dynamic Model `MAGIC' to Predict Recovery Following Implementation of the Gothenburg Protocol

Reduction of sulphur deposition causesrecovery of acidified surface waters. Processes in thecatchment delay recovery. The acidification model MAGICwas applied to the Vikedal and Tovdal rivers in southernNorway. Response in water chemsitry is delayed by 10–20 yr. The delay is due to release of old sulphate atVikedal and cation exchange at Tovdal. Assuming that theGothenburg protocol is fully implemented by the year2010, much of the predicted increase of ANC will occur inthe next 10 yr with a levelling off by about 2040. Ifnitrogen leaching increases in the future, however,recovery of ANC will not be as rapid, nor as complete.Critical load for acidity calculated by steady-statemodels is confirmed by the MAGIC predictions. Futurerequirement for mitigation measures such as liming willdecrease in the future as acid deposition decreases. Bythe year 2046 the liming requirement will be reduced byabout 45% at Vikedal and 65% at Tovdal. One of the mainpurposes of the Norwegian national monitoring programmeis to provide documentation of changes in environmentalquality due to long-range transported air pollutants.Modelling applications such as this clearly show that thedata fill this purpose.     

Invasives, Introductions and Acidification: The Dynamics of a Stressed River Fish Community

We describe the development of the fish community in the acidified and limed river Litleåna in southern Norway, and describe how chemical restoration, compensatory introductions of exotics, and accidental invasion of exotics interact to influence the population of the naturally occurring brown trout (Salmo trutta). The river Litleåna is a tributary to the river Kvina in Vest-Agder County, southern Norway. During the years 1996–2004, annual mean pH was 4.9–5.0 and 6.1–6.4 above and below the liming facility, which was installed in 1994. Originally, brown trout was the only fish species in the river, but brook trout (Salvelinus fontinalis) have been intentionally introduced, whereas European minnow (Phoxinus phoxinus) was introduced by accident. Fish densities were recorded by means of electrofishing annually over the ten year period 1995–2004. Although close to extinction before liming was initiated, brown trout fry densities increased from 1995 to 1999, with subsequent varying densities. There has been a simultaneous major increase in the occurrence and density of European minnow since 1997. Our results show that both brown trout and European minnow increase after liming. Minnow densities are negatively affected by low pH episodes in the river. The growth rates of brown trout fry are negatively correlated to minnow densities, indicating competition between the species. Brook trout densities have decreased since liming started, and during the brown trout recovery.     

Nitrate Leaching from Moorland Soils: Can Soil C:N Ratios Indicate N Saturation?

Links between forest floor carbon:nitrogen (C:N) ratios, atmospheric N deposition and nitrate leaching into surface waters have been reported for forest ecosystems, but similar studies have not been reported previously for the equivalent compartments of moorland ecosystems in Great Britain, despite the importance of nitrate in contributing to the acidification of moorland streams and lakes in British uplands. In this paper, the relationships between the C:N ratio of moorland soil surface organic matter, N deposition, and nitrate leaching are explored for 13 soils in four moorland catchments. Although there is spatial variability in the C:N ratio of soils, major differences are apparent between soils and especially between catchments. The C:N ratio appears to be inversely related to modelled inorganic N deposition and, to a lesser degree, measured nitrate leaching, for three of the four catchments studied (Allt a'Mharcaidh, Afon Gwy, and Scoat Tarn). Nitrification may make an important contribution to nitrate leaching at the two higher deposition sites. At the fourth site, the heavily acidified River Etherow catchment, extremely high rates of nitrate leaching are not accompanied by low C:N ratios or high nitrification potentials in the upper soil horizons. Hence the C:N ratio of surface soil organic matter may have potential as an indicator of nitrogen saturation and leaching in some systems, but it is not universally applicable.     

A Novel Environmental Quality Criterion for Acidification in Swedish Lakes – An Application of Studies on the Relationship Between Biota and Water Chemistry

The recovery from acidification has led to the demand for more precise criteria for classification of acidification. The Swedish Environmental Protection Agency has revised Sweden’s Ecological Quality Criteria for acidification to improve the correlation between the chemical acidification criteria and biological effects. This paper summarises the most relevant findings from several of the studies commissioned for this revision. The studies included data on water chemistry in 74 reference lakes in southern Sweden with data on fish in 61 of the lakes, as well as data on littoral fauna in 48 lakes. We found that the acidity variable most strongly correlated to the biota was the median pH from the current year. Our results probably do not reflect the mechanisms behind the negative effects of acidity on the biota, but are fully relevant for evaluation of monitoring data. The biogeochemical models used for predicting acidification reference conditions generate a pre-industrial buffering capacity. In order to get an ecologically more relevant criteria for acidification based on pH, we transferred the estimated change in buffering capacity into a corresponding change in pH. A change of 0.4 units was defined as the threshold for acidification. With this criterion a considerably lower number of Swedish lakes were classified as acidified when compared with the present Ecological Quality Criteria.     

Dynamics of P, Al, and Fe during High Discharge Episodic Acidification at the Bear Brook Watershed in Maine, U.S.A.

Phosphorus (P), aluminum (Al), and iron (Fe) stream chemistry were assessed for high discharge snowmelt events at the Bear Brook Watershed, Maine (BBWM) during December 2001 and February 2002 and compared with results from a January 1995 study of the same streams. The West Bear catchment has been subjected to artificial acidification since 1989. The East Bear catchment is the untreated reference. Total (acid soluble) Al, Fe, and P were positively correlated with discharge during the 2001–2002 events. However, dissolved P concentrations remained low (≤0.1 μmol L^-1) during high discharge events as pH decreased in both streams.For example, in 2001, total P concentration increased to 1.7 μmol L^-1 during the rising limb of the hydrograph in West Bear, approximately five times the value in East Bear. During the same event, in West Bear and East Bear dissolved Al concentrations increased to 21 and 6.3 μmol L^-1, respectively, while total Al concentrations increased to 166 and 30 μmol L^-1, respectively. Dissolved Fe concentrations remained ≤0.9 μmol L^-1 in both streams during all study events. However, total Fe concentrations in 2001 increased to 239 and 4.1 μmol L^-1 for West Bear and East Bear, respectively. Total Al and Fe declined parallel to total P after peaking during all study periods. Nearly all of the base cations were in dissolved form during the three events, indicating that total Al in West and East Bear Brooks is not associated with primary minerals such as feldspars. We conclude that particulate Al, Fe, and P are chemically linked during transport at high discharge in these episodically and chronically acidified streams.     

Modelling Acidification and Recovery of Swedish Lakes

The MAGIC model was calibrated to 143 lakes in Sweden, all of which are monitored in Swedish national monitoring programmes conducted by the University of Agricultural Sciences (SLU). Soil characteristics of the lake catchments were obtained from the National Survey of Forest Soils and Vegetation also carried out by SLU. Deposition data were provided by the Swedish Meteorological and Hydrological Institute (SMHI). The model successfully simulated the observed lake and soil chemistry at 133 lakes and their catchments. The fact that 85% of the lakes calibrated successfully without being treated in an individual way suggests that data gathered by the national monitoring programmes are suitable for modelling of soil and surface water recovery from acidification. The lake and soil chemistry data were then projected into the future under the deposition scenario based on emission reductions agreed in the Gothenburg protocol. Deposition of sulphur (sea salt corrected) was estimated to decrease from 1990 to 2010 by 65–73%; deposition of nitrogen was estimated to decrease by 53%. The model simulated relatively rapid improvements in lake water chemistry in response to the decline in deposition from 1990 to 2010, but the improvements levelled off once deposition stabilised at the lower value. There was a major improvement of simulated lake water charge balance acid neutralising capacity (ANC) from 1990 to 2010 in all lakes. The modelled lakes were divided into acidification sensitive and non-sensitive. The modelled sensitive lakes are representative of 20% of the most sensitive lakes in Sweden. By 2010, the ANC in the sensitive lakes was 10 to 50 μeq L^-1 below estimated pre-industrial levels and did not increase much further from 2010 to 2040. Soils at the majority of the modelled catchments continued to lose base cations even after the simulated decline in acid deposition was complete, i.e. after the year 2010. Based on this model prediction, the acidification of the Swedish soils will in general not be reversed by the deposition reduction experienced over the last 10 years and expected to occur by the year 2010.     

A conceptual model of spatially heterogeneous nitrogen leaching from a welsh moorland catchment

Soil- and stream-water data from the Plynlimon research area, mid-Wales, have been used to develop a conceptual model of spatial variations in nitrogen (N) leaching within moorland catchments. Extensive peats, in both hilltop and valley locations, are considered near-complete sinks for inorganic N, but leach the most dissolved organic nitrogen (DON). Peaty mineral soils on hillslopes also retain inorganic N within upper organic horizons, but a proportion percolates into mineral horizons as nitrate (NO^? ₃), either through incomplete immobilisation in the organic layer, or in water bypassing the organic soil matrix via macropores. This NO^? ₃ reaches the stream where mineral soilwaters discharge (via matrix throughflow or pipeflow) directly to the drainage network, or via small N-enriched flush wetlands. NO^? ₃ in hillslope waters discharging into larger valley wetlands will be removed before reaching the stream. A concept of catchment ‘nitrate leaching zones’ is proposed, whereby most stream NO^? ₃ derives from localised areas of mineral soil hillslope draining directly to the stream; the extent of these zones within a catchment may thus determine its overall susceptibility to elevated surface water NO^? ₃ concentrations.     

Sediment–Water Interactions in an Eroded and Heavy Metal Contaminated Peatland Catchment,Southern Pennines,UK

Atmospherically deposited lead in the upper layer of the heavily eroded peatlands of the Peak District, southern Pennines, UK, reaches concentrations in excess of 1,000 mg kg⁻¹. Erosion of the upper peat layer in this region is releasing lead, associated with eroded peat particles, into the fluvial system. Understanding the process mechanisms that control dissolved lead concentrations in contaminated peatland streams is vital for understanding lead cycling and transport in peatland streams. Many headwater streams of the southern Pennines recharge drinking water reservoirs. Measurements in the Upper North Grain (UNG) study catchment show that mean sediment-associated and dissolved lead concentrations are 102 ± 39.4 mg kg⁻¹ and 5.73 ± 2.16 μg l⁻¹, respectively. Experimental evidence demonstrates that lead can desorb from suspended sediments, composed of contaminated peat, into stream waters. In-stream processing could therefore account for the elevated dissolved lead concentrations in the fluvial system of UNG.     

Fish Stomachs as a Biomonitoring Tool in Studies of Invertebrate Recovery

High mortality rates due to predation from fish may reduce densities of preferred prey animals. Predation may also depress the rate of recovery from environmental stress. In an alpine ecosystem damaged by acidification, we compared three different techniques of monitoring the recovery of two large species of crustaceans, the amphipod Gammarus lacustris and the notostrachan Lepidurus arcticus. The methods used were: (1): benthic littoral kick samples, (2): artificial substrate in the form of jute bags, (3): examination of brown trout stomachs. The monitoring took place in two limed lakes at the Hardangervidda mountain plateau in Central Norway, L. Svartavatn and L. Svartavasstjørni. Brown trout, Salmo trutta, is the only fish species in the lakes. Liming as a water quality improvement measure was started in 1994. All stomach samples were negative with respect to Gammarus and Lepidurus during the period 1987–1998. In 1999, the first records of both species were done in trout stomachs collected from Lake Svartavatnet. In Lake Svartavasstjørni, Lepidurus and Gammarus reappeared in fish stomachs in 2001 and 2002, respectively. During the period of monitoring, no records of these crustaceans were done in benthic samples and on artificial substrate in any of the two lakes. In an unacidified reference site, Lake Skiftesjøen, both benthic samples and the jute bags indicated a dense population of Gammarus. Our results strongly indicate that studies of fish stomachs are the best method for monitoring low-density populations of attractive fish food animals.     

A Conceptual Model of Spatially Heterogeneous Nitrogen Leaching from a Welsh Moorland Catchment

Soil- and stream-water data from the Plynlimon research area, mid-Wales, have been used to develop a conceptual model of spatial variations in nitrogen (N) leaching within moorland catchments. Extensive peats, in both hilltop and valley locations, are considered near-complete sinks for inorganic N, but leach the most dissolved organic nitrogen (DON). Peaty mineral soils on hillslopes also retain inorganic N within upper organic horizons, but a proportion percolates into mineral horizons as nitrate (NO ₃ ^– ), either through incomplete immobilisation in the organic layer, or in water bypassing the organic soil matrix via macropores. This NO ₃ ^– reaches the stream where mineral soilwaters discharge (via matrix throughflow or pipeflow) directly to the drainage network, or via small N-enriched flush wetlands. NO ₃ ^– in hillslope waters discharging into larger valley wetlands will be removed before reaching the stream. A concept of catchment nitrate leaching zones is proposed, whereby most stream NO ₃ ^– derives from localised areas of mineral soil hillslope draining directly to the stream; the extent of these zones within a catchment may thus determine its overall susceptibility to elevated surface water NO ₃ ^– concentrations.     

Controls on leaching of N species in upland moorland catchments

Spatial and temporal changes in mobility of N species have been studied for three UK upland river networks, the Etherow in the South Pennines, the Nether Beck in the Lake District and the Dee in NE Scotland. The catchments are subject to N deposition at 35.1, 22.0 and 10.8–15.6 kg N ha^?1 yr^?1, respectively. The NH⁺ ₄ leaching appears to be predominantly regulated by flow path in more polluted upland catchments. It is greatest where water draining acidified peaty soils contributes more to total discharge. Soluble organic matter may provide the dominant counter anion. In the Etherow and Dee catchments, which are dominated by acid mineral and organic soils, at high discharge NO^? ₃ also appears to be associated with greater input of water from acidified soils. In contrast, for the Nether Beck, higher NO^? ₃ concentrations are associated with tributaries draining soils contributing water with higher alkalinity, suggesting nitrification is important. For the Etherow and Dee, dissolved organic N (DON) appears to originate predominantly from acidified, peaty soils. Spiking experiments with peat soil from the Etherow catchment confirmed the limited capacity of these soils to utilize inorganic N inputs, favouring equilibration with NH⁺ ₄ inputs and leaching losses of inorganic N throughout the year.     

Recovery of Acidified Lakes: Lessons From Sudbury, Ontario, Canada

Over 7,000 lakes around Sudbury, Ontario, Canada were acidified by S deposition associated with emissions from the Sudbury metal smelters and more distant S sources. Air pollution controls have led to widespread changes in damaged Sudbury lakes, including increased pH and decreased concentrations of SO₄, metals and base cations. While chemical improvements have often been substantial, many lakes are still acidified, although water quality recovery is continuing. Biological recovery has been observed in some lakes among various groups of organisms including fish, zooplankton, phytoplankton and zoobenthos. Generally, however, biological recovery is still at an early stage. Lakes around Sudbury are also showing that the recovery of acid-damaged lakes is closely linked to the effects of other major environmental stressors such as climate change, base cation depletion and UV-B irradiance. Future studies of the recovery of acid-damaged lakes around Sudbury, and in other regions, will need to consider the interactions of these and other stressors.     

Controls on Leaching of N Species in Upland Moorland Catchments

Spatial and temporal changes in mobility of N species have been studied for three UK upland river networks, the Etherow in the South Pennines, the Nether Beck in the Lake District and the Dee in NE Scotland. The catchments are subject to N deposition at 35.1, 22.0 and 10.8–15.6 kg N ha^–1 yr^–1, respectively. TheNH ₄ ⁺ leaching appears to be predominantly regulated by flowpath in more polluted upland catchments. It is greatest where water draining acidified peaty soils contributes more to total discharge. Soluble organic matter may provide the dominant counter anion. In the Etherowand Dee catchments, which are dominated by acid mineral and organic soils, at high discharge NO ₃ ^– also appears to be associated with greater input of water from acidified soils. In contrast, for the Nether Beck, higher NO ₃ ^– concentrations are associated with tributaries draining soils contributingwater with higher alkalinity, suggesting nitrification is important. For the Etherow and Dee, dissolved organic N (DON) appears to originate predominantly from acidified, peaty soils. Spiking experiments with peat soil from the Etherow catchment confirmed the limited capacity of these soils to utilize inorganic N inputs, favouring equilibration with NH ₄ ⁺ inputs and leaching losses of inorganic N throughout the year.     

Temporal Trends in Water Chemistry in the Turkey Lakes Watershed Ontario,Canada, 1982-1999

The Turkey Lakes Watershed (TLW) was established in 1980 as asite for study of the ecosystem effects of acidic deposition, andsince then there has been 40% reduction in North AmericanSO₂ emissions. Monitoring records for bulk deposition,shallow and deep ground water, two headwater streams and two lakeoutflows have been tested to identify statistically significantmonotonic trends. The TLW appears to be responding to decliningacidifying emissions because the most prevalent chemical trendacross sample types/stations was decreasing SO₄ ^2-. Increasing pH was detected in four of the seven data sets, butonly the H⁺ decrease in bulk deposition was of a magnitudeto be an important ionic compensation for the SO₄ ^2-decline. There is little evidence of acidification recovery inTLW waters however. Increasing alkalinity was found only in theoutflow of the penultimate lake of the basin, and in fact, deepground water and the other lake outflow had decreasing alkalinitytrends (i.e., continuing acidification). For the surface waterstations, the greater part of the ionic compensation fordeclining SO₄ ^2- was decreasing base cations, and as aresult, these waters are probably becoming more dilute with time,although only the headwater streams exhibited decliningconductivity. Five of seven data sets had increasing dissolvedorganic carbon concentrations. Increasing NO₃ ^- wasimportant in ground waters. Drought has strongly influencedtrends and delayed recovery by mobilizing S stored in catchmentwetlands and/or soils.     

Incorporation of Seasonal Nitrogen Dynamics within a Long-Term Acidification Model

This paper describes an application of the long termdynamic model, MAGIC, on a monthly timestep, enablingincorporation of the seasonal dynamics associated with abroad understanding of the ecosystem N cycle. The modelhas been applied to the Dargall Lane catchment in theGalloway region of Scotland where marked seasonal Ndynamics are apparent. Mean monthly proportions ofrainfall, runoff, deposition fluxes and net retention ofN are utilised to drive the model on a monthly timestep.Calibration of the model has successfully reproduced thepresent day observed seasonal variation in streamNO₃ and ANC. Prediction of recovery at the siteunder the second sulphur protocol indicates that,although mean annual ANC increases, mean monthly ANC doesnot rise above zero for all months of the year until2010.     

Trends in the Water Chemistry of High Altitude Lakes in Europe

Here we present the chemical trends of seven high altitude lakes, analysed within the AL:PE and MOLAR Projects of the EU (1999) and selected on the basis of the availability of complete and reliable data for the period 1984–1999. The lakes are representative of the Scandinavian Alps, the Cairngorm Mountains in Scotland, the Alps and the Pyrenees. Significant trends were identified for some indicators of acidification, for instance pH and alkalinity, but not all lakes reacted similarly to decreasing depositions of sulphate and base cations. Differences in lake response are discussed in relation to recent variations of atmospheric deposition chemistry and associated changes in climatic conditions. Beside individual variations of the studied lakes, depending, among other things, on altitude and morphology, catchment characteristics and climate trends play a major role for the reaction of high altitude lakes on changes in atmospheric depositions.     

The importance of chemical buffering for pelagic and benthic colonization in acidic waters

In poorly buffered areas acidification may occur for two reasons: through atmospheric deposition of acidifying substances and – in mining districts – through pyrite weathering. These different sources of acidity lead to distinct clearly geochemistry in lakes and rivers. In general, the geochemistry is the major determinant for the planktonic composition of the acidified water bodies, whereas the nutrient status mainly determines the level of biomass. A number of acidic mining lakes in Eastern Germany have to be neutralized to meet the water quality goals of the European Union Directives and to overcome the ecological degradation. This neutralization process is limnologically a short-term maturation of lakes, which permits biological succession to overcome two different geochemical buffer systems. First, the iron buffer system characterizes an initial state, when colonization starts: there is low organismic diversity and productivity, clear net heterotrophy in most cases. Organic carbon that serves as fuel for the food web derives mainly from allochthonous sources. In the second, less acidic state aluminum is the buffer. This state is found exceptionally among the hard water mining lakes, often as a result of deposition of acidifying substances onto soft water systems. Colonization in aluminum-buffered lakes is more complex and controlled by the sensitivity of the organisms towards both, protons and inorganic reactive aluminum species. In soft-water systems, calcium may act as antidote against acid and aluminum; however, this function is lost in hard water post mining lakes of similar proton concentrations. Nutrient limitations may occur, but these do not usually control qualitative and quantitative plankton composition. In these lakes, total pelagic biomass is controlled by the bioavailability of nutrients, particularly phosphorus.     

Acidification Trends and the Evolution of Neutralization Mechanisms through Time at the Bear Brook Watershed in Maine (BBWM), U.S.A.

The paired catchment study at the forested Bear Brook Watershed in Maine (BBWM) U.S.A. documents interactions among short- to long-term processes of acidification. In 1987–1989, runoff from the two catchments was nearly identical in quality and quantity. Ammonium sulfate has been added bi-monthly since 1989 to the West Bear catchment at 1800 eq ha^-1 a^-1; the East Bear reference catchment is responding to ambient conditions. Initially, the two catchments had nearly identical chemistry (e.g., Ca²⁺, Mg²⁺, SO₄ ^2-, and alkalinity ≈82, 32, 100, and 5 μeq L^-1, respectively). The manipulated catchment responded initially with increased export of base cations, lower pH and alkalinity, and increased dissolved Al,NO₃ ^- and SO₄ ^2-. Dissolved organic carbon and Si have remained relatively constant. After 7 yr of treatment, the chemical response of runoff switched to declining base cations, with the other analytes continuing their trends; the exports of dissolved and particulate Al, Fe, and P increased substantially as base cations declined. The reference catchment has slowly acidified under ambient conditions, caused by the base cation supply decreasing faster than the decrease of SO₄ ², as pollution abates. Export of Al, Fe and, P is mimicking that of the manipulated watershed, but is lower in magnitude and lags in time. Probable increasing SO₄ ^2- adsorption caused by acidification has moderated the longer-term trends of acidification of both watersheds. The trends of decreasing base cations were interrupted by the effects of several short-term events, including severe ice storm damage to the canopy, unusual snow pack conditions, snow melt and rain storms, and episodic input of marine aerosols. These episodic events alter alkalinity by5 to 15 μeq L^-1 and make it more difficult to determine recovery from pollution abatement.     

Stem Growth of Picea Abies in South Western Sweden in the 10 Years Following Liming and Addition of PK and N

Liming and/or application of specific nutrients have been proposed as countermeasures to the acidification of forest soils in southern Sweden. In this study the stem growth of Picea abies (L.) Karst. growing on acidic mineral soils in SW Sweden was investigated 10 years after additions of lime (Ca; 3000 kg lime ha⁻¹), lime plus P (25 kg ha⁻¹) and K (80 kg ha⁻¹), or N in low doses (2 × 10 kg ha⁻¹ yr⁻¹) (treatments: CaPK, Ca, N, CaPKN, and 2Ca2P2K, respectively). Compared with the control, stem growth was increased following all treatments involving lime additions, including liming alone. The PK addition did not seem to affect growth. The most plausible cause of the observed growth increases was that the lime additions indirectly increased the supply of plant-available N. The annual low-dose N addition did not significantly affect growth. This suggests that air-borne deposition of N, which supplies very small doses of N throughout the year, has a minor or even negligible influence on P. abies growth.     

A Comparison of Loch Chemistry from 1955 and 1999 in the Cairngorms,N.E. Scotland

The Cairngorms in north-east Scotland is remote from pollutant sources although it currently receives ca. 10 kg ha¹ yr¹ S and ca. 11 kg ha¹ yr¹ N deposition from the atmosphere.In 1955, 15 lochs (lakes) at a range of altitudes were sampled and analysed for major ion concentrations. A new survey of these and an additional 23 lochs and their catchment soils was conducted in 1999 to determine the impact of acid deposition, and the changes in loch chemistry since the 1955 survey. The bedrock geology of this region has a strong influence on the loch chemistry. Surface waters were generally more acidic in high altitude areas due to predominantly poorly buffered, thin alpine soils developed on granitic parent material (mean acid neutralising capacity (ANC) for 23 lochs = 30 eq L¹). At lower altitudes where the geology is dominated by Dalradian metamorphic rocks surface waters are comparatively base rich and have higher ANC (mean ANC for 15 lochs = 157 eq L¹). Surface water nitrate concentrations show a negative relationship with soil C:N status, in that higher nitrate only occurs at low soil C:N ratios. A comparison of data for 1955 and 1999 shows that sulphate concentrations are significantly lower (67.8 and 47.5 eq L¹, respectively), and pH has improved (pH 5.6 and 5.9) in response to decreased S deposition since the mid 1970s. However, mean nitrate concentrations were found to increase from 2.48 >eq L¹ in 1955 to 5.65 eq L¹ in 1999. Differences in the sampling and laboratory methods from 1955 and 1999 are acknowledged in the interpretation of data.