Predicting Freshwater Critical Loads from Catchment Characteristics using National Datasets

Maps of freshwater critical loads are used toguide emission strategies for sulphur and nitrogen bothnationally and internationally. Water chemistry data arerequired to calculate critical loads and the production ofnational maps therefore relies on the existence of extensivechemistry datasets. However, the data required to calculatecritical loads are not readily available for all sites. Thisarticle explores how empirical statistical models mightpotentially be used to predict critical loads using nationallyavailable datasets representing a range of catchmentcharacteristics. Initially a global regression model forexplaining freshwater critical load variation across a broadspectrum of catchment types (from lowland agricultural tomountain lakes) throughout mainland Britain is described. Whenattention is focused on more specific catchment types (i.e.upland and non-arable) it is shown that the global model hasless explanatory power. A regionalisation of Great Britain(based on 100 km grid squares) shows that the global modelcannot necessarily be applied successfully within a narrowerregional context. Separate analyses were undertaken on each ofthe regional subsets using backward selection regression. Thevariables emerging as significant predictors variedsubstantially across the regions, as did the explanatory powerof the models. This was also the case when the analysis wasconfined to upland and non-arable catchments. This approachcould be developed so that critical loads assessments can bemade for populations of standing waters rather than simplythose for which water chemistry is available.     

The Input and Transmission of Fallout Radionuclides Through Redó, a High Mountain Lake in the Spanish Pyrenees

Fallout radionuclides have increasing value as tracers of pathways for pollutant transport through catchment/lake systems, in addition to their more traditional role in dating sediment records. The objectivesof this study, carried out within the EU MOLAR project, were tomeasure atmospheric fluxes of fallout ²¹⁰Pb, ¹³⁷Cs and ⁷Be at Redó, to establish mass balances for theseradionuclides, and test and validate models of pollutant transport through the lake and its catchment. This was achieved by comparing measured fluxes and concentrations in the water column with theoretical estimates using simple compartment models. Several interesting points emerged. Differences betweensoil core and rainwater measurements suggest that Saharan dust may be an important source of fallout ²¹⁰Pb. Fluxes throughthe water column had a clear seasonal trend reflecting winter icecover. Significant concentrations of ¹³⁷Cs are still presentin the water column, due to continued inputs from the catchment and/or remobilisation from the bottom sediments.     

Element Removal in Harvested Tree Biomass: Scenarios for Critical Loads in Wallonia,South Belgium

The critical load concept is nowwidely used as a tool for developing emissioncontrol policies in Europe. As a signatorycountry of the Convention of Long-RangeTransboundary Air Pollution, critical loads foracidity, nutrient nitrogen, nitrogen and sulphurhave been calculated for the Flemish and Walloonregions in Belgium. This paper describes themethodology used for estimating critical loadsfor forest soils in the Walloon region accordingto the Steady-State Mass Balance equations. As anexample the methodology was applied to thecatchment `Waroneu', situated in a sensitive areaof the Haute Ardenne. Main input parameters tothe equations were derived from precipitation andrunoff data of the catchment study. Improvedestimates of nitrogen uptake (Nu) and base cationuptake (BCu) were obtained by intensive samplingof Picea abies and Quercus roburtrees. Nutrient contents (Ca, Mg, K, N) andnutrient to nitrogen ratios of Picea abiesreflected the poor soil quality at a site withhigh N deposition. Quercus robur nutrientcontents increased from stem to higher orderbranches with a high proportion of nutrientslocated in the bark. However the simulation ofstem only harvesting had a minor effect oncritical loads. Measured wood densities werelower than reported literature values with a maineffect on Nu and BCu estimates. The use ofrecommended default values and/or data derivedfrom the experimental site resulted in a widerange of critical loads, some of which werelargely overestimated. Results demonstrated theimportance of site specific data for criticalload calculations.     

Wildfire Effects on the Quantity and Composition of Suspended and Gravel-Stored Sediments

In August of 2003 a severe wildfire burnt the majority of Fishtrap Creek, a 170 km² catchment in central British Columbia, Canada. The objective of this study was to determine the short-term (15-month) influence of the wildfire on the amount and composition of fine sediment delivery and retention in the system and to compare it to a similar unburnt catchment. In the spring of 2004 automatic water samplers were installed at a gauging site on Fishtrap Creek to collect suspended sediments from the snowmelt runoff and gravel traps were deployed on the channel bed surface to collect composite samples of suspended fine sediment. Jamieson, the reference creek, exhibits similar geology and pre-burn vegetation and was sampled in the same manner for comparison. Composite suspended sediment collected in the traps was removed from the streams in mid-summer and early September. Quantitative estimates of the amount and particle size structure of the naturally stored fine sediment in, and on, the gravel creekbed were obtained in pre-melt, mid and late-summer conditions. Estimates of suspended sediment yields indicated that while the burnt system delivered 66% more material per unit area, the total seasonal suspended sediment yield was low (855 kg km⁻²) compared to other fire-disturbed systems. While the burnt catchment was primed to deliver sediment, the hydrologic drivers were not of sufficient magnitude to generate a substantial response, suggesting that in this first post-fire year the system was transport-limited, not supply-limited. Differences were noted in the spatial and seasonal composition of the <500 more OM% composite suspended sedimentswith the burnt catchment having significantly (P≤0.05) more OM%. Seasonally a significant increase of OM% in late summer samples was associated with instream biofilms and possible delivery of black carbon. The system’s post-fire response was not geomorphically substantial but significant biological differences were noted in the short-term.     

Development and Application of Critical,Target and Monitoring Loads for the Management of Acid Deposition in Alberta,Canada

The Alberta, Canada acid deposition management framework, based upon the application of critical, target and monitoring loads, is described. This framework is the culmination of four years work by stakeholders brought together within Alberta's Clean Air Strategic Alliance (CASA). The elements of the framework include scientific aspects of measurement, model estimation, and monitoring of acid deposition, assessment of receptor sensitivity, and management processes to reduce emissions and deposition (should reductions become necessary). All loads are applied to grid cells measuring 1°latitude × 1° longitude, with each cell being categorized as sensitive, moderately sensitive or of low sensitivity on the basis of the sensitivities of the soil and water systems within the cell. Critical loads have been set at 0.25, 0.50 and 1.00 keq H⁺ ha^-1 yr^-1 for grid cells that are categorized as sensitive, moderately sensitive, and of low sensitivity, respectively. Target loads, the environmental management objectives, have been set at 0.22, 0.45, and 0.90 keq H⁺ ha^-1 yr^-1, and monitoring loads, a new concept in acid deposition management, have been set at 0.17, 0.35 and 0.70 keq H⁺ ha^-1 yr^-1 for the three sensitivity classes. When model prediction indicates that deposition may be exceeding the monitoring load, deposition monitoring and receptor sensitivity studies are to be initiated to confirm the deposition model prediction, and to ensure that the sensitivity of the recipient systems is understood. In this manner, management actions that occur in the event of a target load exceedance will be based upon receptor sensitivity and deposition data rather than upon model prediction alone. A process for stakeholder involvement in the evaluation of the framework and its application in long-term, long-range management of emissions and deposition is also included within the framework.     

Deposition Loads of Sulphur and Nitrogen in Germany

High spatial resolution maps of deposition loads in Germanyare produced as an input for abatement strategy research andfor critical loads exceedance calculations on a nationalscale. In this paper methods ofmapping total deposition loads in Germany and preliminarymaps of nitrogen and sulphur deposition loads for the year1993 are presented. A comparison of these mapping resultswith EMEP deposition mapping results has been carried out.The differences in the results of the German national and theEuropean EMEP mapping, due to different databases anddifferent methods, are quantified and discussed. Highresolution maps of deposition loads are compared to Europeanlow resolution maps on the same temporal and spatial scale,assuming that on average both should lead to similar results.However, the average differencescalculated for 23 EMEP 150 × 150 km² grid cells over Germanywere found to be 33% higher for sulphur (S) total depositionby the German method 65% higher for S dry deposition and1% lower for S wet deposition. The German results fornitrogen (N) total deposition are 2% higher than the EMEPresult 22% higher for N dry deposition and 10% lower for Nwet deposition.     

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.     

Critical Loads of Acidity for Surface Waters in South-Central Ontario, Canada: Regional Application of the First-Order Acidity Balance (FAB) Model

Major sulphur emission control programs have been implemented in North America, resulting in current emissions being ～30% less than those in 1980. However, the level of acidic deposition remaining is still unlikely to promote widespread recovery of aquatic ecosystems. The First-order Acidity Balance (FAB) model has been applied to south-central Ontario (285 lakes in the Muskoka River Catchment) to evaluate the need for further reductions in emissions. As a result of the past decline in deposition, the proportion of lakes with critical loads exceedance has dropped substantially; however, further reductions in sulphur and nitrogen emissions are required to eliminate critical loads exceedance. Based on bulk deposition of sulphate and nitrogen (41.1 mmol_c m^-2 yr^-1 and 62.5 mmol_c m^-2 yr^-1, respectively) for the period 1995–1999, 166 lakes (58.3%) exceedcritical loads. Even with full implementation of SO₂ abatementprograms in Canada (achieved in 1994) and the United States (legislated for 2010), critical loads will be exceeded in a large proportion (46.6%) of the study lakes.     

Effects of Soil Moisture Variations on Deposition Velocities Above Vegetation

The parameterized subgrid-scale surface flux (PASS) modelprovides a simplified means of using remote sensing data from satellites and limited surface meteorological information to estimate the influence of soil moisture on bulk canopy stomatalresistances to the uptake of gases over extended areas.PASS-generated estimates of bulk canopy stomatal resistance were usedin a dry deposition module to compute gas deposition velocitieswith a horizontal resolution of 200 m for approximately 5000 km² of agricultural crops and rangeland. Results were compared with measurements of O₃ flux and concentrations made during April and May 1997 at two surface stations and from an aircraft. The trend in simulated O₃ deposition velocityduring soil moisture drydown over a period of a few days matchedthe trend observed at the two surface stations. For areas underthe aircraft flight paths, the variability in simulated O₃ deposition velocity was substantially smaller than the observedvariability, while the averages over tens of kilometers were usually in agreement within 0.1 cm s^-1. Model results indicated that soil moisture can have a major role in depositionof O₃ and other substances strongly affected by canopy stomatal resistance.     

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.     

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.     

Freshwater Critical Loads in Wales

The Steady State Water Chemistry (SSWC) modeland the Diatom model have been used to calculate criticalloads for acidity using annual mean chemistry for 102 acidupland streams in Wales sampled as part of the Welsh AcidWaters Survey (WAWS) in 1995. Diatom critical loads werelower than SSWC values reflecting the higher effective[ANC]_limit of the Diatom model compared to the[ANC]_limit of zero used in the SSWC model. The WAWSstream sites were all located within 41 10 × 10 km squares andeach square was assigned the lowest critical load value fromamongst the sites located within it. Comparison with valuesassigned under the UK national critical loads mappingprogramme (UKCLMAP) showed that WAWS critical loads were lowerthan UKCLMAP values in approximately 40% of squares.Differences in critical load class were variable, but exceeded2 keq ha^-1 yr^-1 in up to a maximum of seven squares.It cannot be assumed, therefore, that reducing acid depositionto the currently mapped UKCLMAP critical load will protect allstreams occurring within a given 10 × 10 km grid square inWales. The limited number of sample sites means that even inthose squares where all WAWS sites will be protected, theremay be other, more acid sensitive freshwaters with lowercritical loads. This has important implications for theinterpretation and use of critical loads data for regional andlocal environmental planning.     

Determinants of nitrous oxide emission from agricultural drainage waters

Emissions of the powerful greenhouse gas nitrous oxide (N₂O) from agricultural drainage waters are poorly quantified and its determinants are not fully understood. Nitrous oxide formation in agricultural soils is known to increase in response to N fertiliser application, but the response of N₂O in field drainage waters is unknown. This investigation combined an intensive study of the direct flux of N₂O from the surface of a fertilised barley field with measurement of dissolved N₂O and nitrate (NO₃) concentrations in the same field’s drainage waters. Dissolved N₂O in drainage waters showed a clear response to field N fertilisation, following an identical pattern to direct N₂O flux from the field surface. The range in N₂O concentrations between individual field drains sampled on the same day was large, indicating considerable spatial variability exists at the farm scale. A consistent pattern of very rapid outgassing of the dissolved N₂O in open drainage ditches was accentuated at a weir, where increased turbulence led to a clear drop in dissolved N₂O concentration. This study underlines the need for carefully planned sampling campaigns wherever whole farm or catchment N₂O emission budgets are attempted. It adds weight to the argument for the downward revision of the IPCC emission factor (EF₅-g) for NO₃ in drainage waters.     

Deposition and Fate of Lead in a Forested Catchment, Lesni Potok, Central Czech Republic

The deposition of trace elements and their fate in a forest ecosystemhas been monitored at the experimental site, Lesni Potok catchment (LP), with granite bedrock. The catchment is located 30 km ESE from Prague. Annual bulk Pb-deposition flux F_Pb was 3.41 kg km^-2 a^-1 in 1994 and gradually decreased to 0.49 kg km^-2 a^-1 in 2001. The decrease is comparable with those observed in Germany and in the U.S.A. in the 1970s and 1980s. The total sales ban of leaded gasoline in the Czech Republic since January 2001 was accompanied by a pronounced decrease of F_Pb in a single year. The residual Pb-deposition flux is assigned to both the long-range transport of fine-grained vehicular lead aerosol (with a long residence time in the atmosphere) and to theemissions from power plant boilers burning lignite mined in the Czech northwest coal basin. The F_Pb of lead correlates stronglywith those of As, Cd, Cu, Zn and Be, the typical metals in coal fly ash, at two monitored sites. Topsoil horizons contain elevated concentrations of Pb (53–67 mg kg^-1), which are of anthropogenicorigin. Soils in the riparian areas contain increased concentrations of Pb when compared to soils on the hillslope areas. Significant amounts of Pb were found on a stream substrate and Fe-precipitate sampled from the stream. Low concentrations of Pb in bark and bole wood suggest that the uptake of Pb by vegetation is negligible. The very small surface water outputs (average of 0.002 kg km^-2 a^-1) compared to inputs (average of 1.890 kg km^-2 a^-1) from the LP catchment indicate an ongoing accumulation of Pb in a forested landscape.     

Spatial and Temporal Variations in the Sediment Habitat of Ranunculus spp. in Lowland Chalk Streams – Implications for Ecological Status?

Ranunculus spp. are the dominant plants of lowland chalk stream habitats in England. The spatial variability of sediment characteristics (silt–clay, organic matter, total phosphorus and total nitrogen content) within stands of Ranunculus spp. was investigated in 12 rivers in lowland England. Variability was found to be high and there were no discernible differences between samples taken from within Ranunculus and a limited number of samples from bare substrate. For two of these rivers, comparisons were also made between reaches upstream and downstream of waste water treatment works outfalls in terms of the characteristics of the sediments within Ranunculus stands. In one river a clear increase in sediment nutrient, fine and organic material content was observed downstream but in the other there was no consistent difference. Temporal variability was considered for two rivers in the Frome catchment, Dorset, by analysing the monthly variability in sediment organic matter and silt–clay content beneath Ranunculus stands over an annual cycle of growth and die-back. Whilst a clear pattern of fine and organic material retention consistent with seasonal plant growth patterns was evident at one site, the three sites displayed different temporal patterns. This inconsistency is believed to reflect differences in sediment supply at the three sites.     

Spatial variability of soil gas concentration and methane oxidation capacity in landfill covers

In order to devise design criteria for biocovers intended to enhance the microbial oxidation of landfill methane it is critical to understand the factors influencing gas migration and methane oxidation in landfill cover soils. On an old municipal solid waste landfill in north-western Germany soil gas concentrations (10, 40, 90 cm depth), topsoil methane oxidation capacity and soil properties were surveyed at 40 locations along a 16 m grid. As soil properties determine gas flow patterns it was hypothesized that the variability in soil gas composition and the subsequent methanotrophic activity would correspond to the variability of soil properties. Methanotrophic activity was found to be subject to high spatial variability, with values ranging between 0.17 and 9.80 g CH₄ m⁻² h⁻¹_. Considering the current gas production rate of 0.03 g CH₄ m⁻² h⁻¹, the oxidation capacity at all sampled locations clearly exceeded the flux to the cover, and can be regarded as an effective instrument for mitigating methane fluxes. The methane concentration in the cover showed a high spatial heterogeneity with values between 0.01 and 0.32 vol.% (10 cm depth), 22.52 vol.% (40 cm), and 36.85 vol.% (90 cm). The exposure to methane raised the oxidation capacity, suggested by a statistical correlation to an increase in methane concentration at 90 cm depth. Methane oxidation capacity was further affected by the methanotroph bacteria pH optimum and nutrient availability, and increased with decreasing pH towards neutrality, and increased with soluble ion concentration). Soil methane and carbon dioxide concentration increased with lower flow resistance of the cover, as represented by the soil properties of a reduced bulk density, increase in air capacity and in relative ground level.     

The Missing Flux in a 35S Budget for the Soils of a Small Polluted Catchment

A combination of cosmogenic and artificial ³⁵S was used to assess the movement of sulfur in a steep Central European catchment affected by spruce die-back. The Jeze?í catchment, Kru?né Hory Mts. (Czech Republic) is characterized by a large disproportion between atmospheric S input and S output via stream discharge, with S output currently exceeding S input three times. A relatively high natural concentration of cosmogenic ³⁵S (42 mBq L^-1) was found in atmospheric deposition into the catchment in winter and spring of 2000. In contrast, stream discharge contained only 2 mBq L^-1. Consequently, more than 95% of the deposited S is cycled or retained within the catchment for more than several months, while older S is exported via surface water. In spring, when the soil temperature is above 0 °C, practically no S from instantaneous rainfall is exported, despite the steepness of the slopes and the relatively short mean residence time of water in the catchment (6.5 months). Sulfur cycling in the soil includes not just adsorption of inorganic sulfate and biological uptake, but also volatilization of S compounds back into the atmosphere. Laboratory incubations of an Orthic Podzol from Jeze?í spiked with 720 kBq of artificial ³⁵S showed a 20% loss of the spike within 18 weeks under summer conditions. Under winter conditions, the ³⁵S loss was insignificant (<5%). This missing S flux was interpreted as volatilized hydrogen sulfide resulting from intermittent dissimilatory bacterial sulfate reduction. The missing S flux is comparable to the estimated uncertainty in many catchment S mass balances (±10%), or even larger, and should be considered in constructing these mass balances. In severely polluted forest catchments, such as Jeze?í, sulfur loss to volatilization may exceed 13 kg ha^-1 a^-1, which is more than the current total atmospheric S input in large parts of North America and Europe.     

Determinants of nitrous oxide emission from agricultural drainage waters

Emissions of the powerful greenhouse gas nitrous oxide (N₂O) from agricultural drainage waters are poorly quantified and its determinants are not fully understood. Nitrous oxide formation in agricultural soils is known to increase in response to N fertiliser application, but the response of N₂O in field drainage waters is unknown. This investigation combined an intensive study of the direct flux of N₂O from the surface of a fertilised barley field with measurement of dissolved N₂O and nitrate (NO₃) concentrations in the same fields drainage waters. Dissolved N₂O in drainage waters showed a clear response to field N fertilisation, following an identical pattern to direct N₂O flux from the field surface. The range in N₂O concentrations between individual field drains sampled on the same day was large, indicating considerable spatial variability exists at the farm scale. A consistent pattern of very rapid outgassing of the dissolved N₂O in open drainage ditches was accentuated at a weir, where increased turbulence led to a clear drop in dissolved N₂O concentration. This study underlines the need for carefully planned sampling campaigns wherever whole farm or catchment N₂O emission budgets are attempted. It adds weight to the argument for the downward revision of the IPCC emission factor (EF₅-g) for NO₃ in drainage waters.     

Spatially Disaggregated Inventories of Soil NO and N2O Emissions for Great Britain

Estimates of soil N₂O and NOemissions at regional and country scales arehighly uncertain, because the most widely usedmethodologies are based on few data, they do notinclude all sources and do not account forspatial and seasonal variability. To improveunderstanding of the spatial distribution of soilNO and N₂O emissions we have developedsimple multi-linear regression models based onpublished field studies from temperate climates.The models were applied to create spatialinventories at the 5 km² scale of soil NOand N₂O emissions for Great Britain. The N₂O regression model described soilN₂O emissions as a function of soil N input,soil water content, soil temperature and land useand provided an annual N₂O emission of 128 kt N₂O-N yr^-1. Emission rates largerthan 12 kg N₂O-N ha^-1 yr^-1 werecalculated for the high rainfall grassland areasin the west of Great Britain.Soil NO emissions were calculated using tworegression models, which described NO emissionsas a function of soil N input with and without afunction for the water filled pore space. Thetotal annual emissions from both methods, 66 and7 kt NO-N yr^-1, respectively, span the rangeof previous estimates for Great Britain.