Monitoring Studies of Precipitation and Cap Cloud Chemistry at Holme Moss in the Southern Pennines

Weekly collections of samples of precipitation and hill cloudwater have been made at Holme Moss (530 m.a.s.l.) in the southernPennines covering a six-year period (1994–1999). In addition continuous meteorological measurements have been conducted at thesite for a five year period (1995–1999). The concentrations of major ions in the samples have been determined by ion chromatography. Analysis of ion concentrations as a function ofwind direction reveals that the ions with anthropogenic sources (SO₄ ^–, NO₃ ^–, NH₄ ⁺, H⁺) exhibit higher concentrations during easterly wind directions whilst the ions with predominantly marine origins (Na⁺, Cl^–, Ca⁺⁺, Mg⁺⁺, K⁺) have concentrations thatare not significantly dependant on wind direction. Precipitation and cloud deposition are strongly correlated to south-westerly wind directions with a secondary peak occurring for north-easterly directions. Fifty nine per cent of ion deposition by rain was found to occur during wind from the SSW to W sector.The average concentrations of ions in cloud water were found tobe much higher than those in rain (by factors of between 2.5 and4.2). It is thought that the high precipitation and annual deposition of ions by precipitation at Holme Moss is due in partto the enrichment of ion concentrations in precipitation by thescavenging of more concentrated cap cloud droplets (the `seeder-feeder effect'). Comparison with data from a nearby lower level site shows encouraging agreement with the scheme currently used in the U.K. deposition mapping procedure to incorporate the influence of orography on deposition by precipitation.     

A Coupled Land-Surface and Dry Deposition Model and Comparison to Field Measurements of Surface Heat,Moisture, and Ozone Fluxes

We have developed a coupled land-surface and drydeposition model for realistic treatment of surface fluxes ofheat, moisture, and chemical dry deposition within acomprehensive air quality modelling system. A new land-surfacemodel (LSM) with explicit treatment of soil moisture andevapotranspiration and an indirect soil moisture nudging schemehas been added to a mesoscale meteorology model. The new drydeposition model uses the same aerodynamic and bulk stomatalresistances computed for evapotranspiration in the LSM. Thisprovides consistent land-surface and boundary layer propertiesacross the meteorological and chemical components of the system. The coupled dry deposition model also has the advantage of beingable to respond to changing soil moisture and vegetationconditions. Modelled surface fluxes of sensible and latent heatas well as ozone dry deposition velocities were compared to twofield experiments: a soybean field in Kentucky during summer 1995and a mixed forest in the Adirondacks of New York in July 1998.(on assignment to the National Exposure Research Laboratory, U.S. Environmental Protection Agency) (author for correspondence, e-mail(on assignment to the National Exposure Research Laboratory, U.S. Environmental Protection Agency)     

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.     

The Control of SO2 Dry Deposition on to Natural Surfaces by NH3 and its Effects on Regional Deposition

Two years of continuous measurements of SO₂deposition fluxes to moorland vegetation are reported. The mean flux of 2.8 ng SO₂ m^-2 s^-1 is regulated predominantly by surface resistance (r _c) which, even for wet surfaces, was seldom smaller than 100 s m^-1. The control of surface resistance is shown to be regulated by the ratio of NH₃SO₂ concentrations with an excess of NH₃ generating the small surface resistances for SO₂. A dynamic surface chemistry model is used to simulate the effects of NH₃ on SO₂ deposition flux and is able to capture responses to short-term changes in ambient concentrations of SO₂, NH₃ and meteorological conditions. The coupling between surface resistance and NH₃/SO₂ concentration ratios shows that the deposition velocity for SO₂ is regulated by the regional pollution climate. Recent long-term SO₂ flux measurements in a transect over Europe demonstrate the close link between NH₃/SO₂ concentrations and rc (SO₂). The deposition velocity for SO₂ is predicted to have increased with time since the 1970s and imply a 40% increase in v _d at a site at which the annual mean ambient SO₂ concentrations declined from 47 to 3 g m^-3 between 1973 and 1998.     

Deposition Velocities of SO2 and O3 over Agricultural and Forest Ecosystems

The results of field studies that measured the flux anddeposition velocity of SO₂ and O₃ are reported. Three of the studies were over agricultural crops (pasture, corn, and soybean), and two were over forest (a deciduous forest and a mixed coniferous–deciduous forest). In all cases the deposition velocity for SO₂ was higher than that for O₃. Diurnal cycles of SO₂ deposition velocity were similar in shape, but not magnitude for all surfaces; however those for O₃ showed some difference between forest sites where the peak was in the morning, and the agricultural sites where the peak occurred at mid-day. Seasonal cycles of SO₂ were affected by deposition to surfaces when leaves were not active, yet surface conductance is significant, but not for O₃ where stomatal uptake is the primary pathway for deposition.(On assignment to the National Exposure Research Lab., US EPA) (e-mail:     

Study of Bulk and Sub-Event Wet Deposition in Gebze,Turkey

This study presents the chemical composition of bulk deposition during the period of February 1996–May 1997 and the chemical composition of sub-event wet deposition on 13 August 1997 in Gebze. Samples were analyzed for SO₄ ^2-, NO₃ ^-, Cl^-,Ca²⁺, Mg²⁺, K⁺, Na⁺, and NH₄ ⁺ in addition to pH. The source of some ionic components in the bulk deposition such as K⁺ and Ca²⁺ were found to be the terrestrial regions, as expected. The (non-sea Cl^-)/Cl^- ratio of 0.05 suggests that the very large portion of Cl^- in the bulkdeposition was of marine origin. The ratio of (non-sea SO₄ ^2-)/SO₄ ^2- varied between 0.86 and 0.99,indicating that the main source of sulfate was not the sea. It is found that the sulfate and calcium concentrations were highest in summer and lowest in fall. The analysis of bulk deposition also indicated that nearly 24% of the events were acidic (pH < 5.6). During sub-event wet deposition collectedon the same site pH decreased continually, and during the passageof cold front concentrations of Cl^-, SO₄ ^2- and NO₃ ^- increased.     

Detecting the signal of atmospheric N deposition in recent national-scale vegetation change across Britain

Model estimates of NO_y and NH_x deposition across Britain for 1996 (5 km square resolution) were applied as explanatory variables to account for national-scale, fine-grained changes in plant species composition between 1990 and 1998. Plant species data were recorded from up to 27 fixed plots located within a stratified random sample of 596 1 km². The response variable was a cover-weighted Ellenberg fertility score for each plot. Analyses were carried out separately for woodlands, semi-natural grasslands and heaths/bogs. Most of the variation in the botanical response variable occurred between plots within squares and so could not be explained by the model deposition data. NH_x deposition estimates accounted for significant, but small components of between 1 km² variation in the change in Ellenberg score in grasslands (5.6%) and heath/bogs (9.8%) but not woodlands. NO_y deposition estimates were not significantly associated with vegetation change. Linear models provided the best fit and the slope of the relationship was lower for heath/bogs than grasslands. Further signal attribution at sub-kilometre square scales requires the development of fine-grained models of N deposition that can be generalised across regional sampling domains.     

A Chronology of Nitrogen Deposition in the UK Between 1900 and 2000

Measurements of the concentrations of nitrogen compounds in air and precipitation in the UK have been made since the mid-19th century, but no networks operating to common protocols and having traceable analytical procedures were established until the 1950s. From 1986 onwards, a high-quality network of sampling stations for precipitation chemistry was established across the UK. In the following decade, monitoring networks provided measurement of NO₂, NH₃, HNO₃ and a satisfactory understanding of the dry deposition process for these gases allowed dry deposition to be quantified. Maps of N deposition for oxidized and reduced compounds at a spatial scale of 5 km × 5 km are available from 1986 to 2000. Between 1950 and 1985, the more limited measurements, beginning with those of the European Air Chemistry Network (EACN) provide a reasonable basis to estimate wet deposition of NO ₃ ^– –N and NH ₄ ⁺ –N. For the first half of the century, estimates of deposition were scaled with emissions assuming a constant relationship between emission and deposition for each of the components of the wet and dry deposition budget at the country scale. Emissions of oxidized N, which dominated total nitrogen emissions throughout the century, increased from 312 kt N annually in 1900 to a peak of 787 kt for the decade 1980–1990 and then declined to 460 kt in 2000. Emissions of reduced N, largely from coal combustion were about 168 kt N in 1900, increasing to a peak of 263 kt N in 2000 and by now dominated by agricultural sources. Reduced N dominated the deposition budget at the country scale, increasing from 163 kt N in 1900 to 211 kt N in 2000, while deposition of oxidized N was 66 kt N in 1900 and 191 kt N in 2000. Over the century, 68 Mt (Tg) of fixed N was emitted within the UK, 78% as NO _x , while 29 Mt of nitrogen was deposited (43% of emissions), equivalent to 1.2 t N ha^–1, on average, with 60% in the reduced form. Deposition to semi-natural ecosystems is approximately 15 Tg N, equivalent to between 1 and 5 t N ha^–1, over the century and appears to be accumulating in soil. The N deposition over the century is similar in magnitude to the total soil N inventory in surface horizons.     

Quantifying dry NH3 deposition to an ombrotrophic bog from an automated NH3 field release system

Providing an accurate estimate of the dry component of N deposition to low N background, semi-natural habitats, such as bogs and upland moors dominated by Calluna vulgaris is difficult, but essential to relate nitrogen deposition to effects in these communities. To quantify the effects of NH₃ inputs to moorland vegetation growing on a bog at a field scale, a field release NH₃ fumigation system was established at Whim Moss (Scottish Borders) in 2002. Gaseous NH₃ from a line source was released along of a 60 m transect, when meteorological conditions (wind speed >2.5 m s^–1 and wind direction in the sector 180–215°) were met, thereby providing a profile of decreasing NH₃ concentration with distance from the source. In a complementary study, using a NH₃ flux chamber system, the relationships between NH₃ concentrations and cuticular resistances were quantified for a range of NH₃ concentrations and micrometeorological conditions for moorland vegetation. Cuticular resistances increased with NH₃ concentration from 11 s m^–1 at 3.0 g m^–3 to 30 s m^–1 at 30 g m^–3. The NH₃ concentration data and the concentration-dependent canopy resistance are used to calculate NH₃ deposition taking into account leaf surface wetness. The implications of using an NH₃ concentration-dependent cuticular resistance and the importance for refining critical loads are discussed.     

The spatial distribution of ammonia emitted from seabirds and its contribution to atmospheric nitrogen deposition in the UK

Simple bioenergetics models were used to derive annual nitrogen excretion rates of each seabird species occurring at colonies in the UK. These were combined with population distribution data and an estimated fraction of nitrogen volatilized to estimate the spatial distribution of NH₃ emissions from seabird colonies at a 1 km resolution. The effect of these emissions on atmospheric NH₃ concentrations and nitrogen deposition in the UK was assessed using the FRAME atmospheric chemistry and transport model. The total emission of NH₃ from the UK seabird colonies is estimated at 2.7 kt yr^–1. Emissions from seabirds are largely concentrated in remote parts of Britain, where agricultural and other anthropogenic emissions are minimal. Although seabirds account for less than 1% of total UK NH₃ emissions (370 kt yr^–1), their occurrence in remote areas and frequently large colony sizes results in seabirds providing a major fraction of the atmospheric nitrogen deposition for many remote ecosystems.     

Atmospheric Budget of Non-Seasalt Chlorine in the Kanto District,Japan

To evaluate the influence of anthropogenic emission of HCl on the air quality in the Kanto district of Japan, the atmospheric budgetof non-seasalt Cl (nssCl) was analyzed. The Kanto district, which consists of the Tokyo metropolis and the six surrounding prefectures, is the most densely populated region in Japan. The emission intensity of HCl is extremely high compared with those in other regions and most western countries. In this study, the annual wet and dry depositions of nssClwere estimated on a 0.25 × 0.25° grid over the Kanto district based on the concentration monitoring resultsand meteorological data. The budget analysis was conducted by comparing the estimated deposition with the emission of HCl. As a result, the annual total (wet + dry) deposition of nssCl was estimated to be 32 kt yr^-1, which closely agreed with HCl emission (36 kt yr^-1) from waste incineration in this area. The result suggested that the anthropogenic emission of HCl had a significant influence on the air quality and the deposition of acidity in this area.     

The Influence of Atmospheric N Deposition on Nitrous Oxide and Nitric Oxide Fluxes and Soil Ammonium and Nitrate Concentrations

The deposition of atmospheric N to soils provides sources of available N to the nitrifying and denitrifying microbial community and subsequently influences the rate of NO and N₂O emissions from soil. We have investigated the influence of three different sources of enhanced N deposition on NO and N₂O emissions 1) elevated NH₃ deposition to woodlands downwind of poultry and pig farms, 2) increased wet cloud and occult N deposition to upland forest and moorland and 3) enhanced N deposition to trees as NO ₃ ^– and NH ₄ ⁺ aerosol. Flux measurements of NO and N₂O were made using static chambers in the field or intact and repacked soil cores in the laboratory and determination of N₂O by gas chromatography and of NO by chemiluminescence analysis. Rates of N deposition to our study sites were derived from modelled estimates of N deposition, NH₃ concentrations measured by passive diffusion and inference from measurements of the ²¹⁰Pb inventory of soils under tree canopies compared with open grassland. NO and N₂O emissions and KCl-extractable soil NH ₄ ⁺ and NO ₃ ^– concentrations all increased with increasing N deposition rate. The extent of increase did not appear to be influenced by the chemical form of the N deposited. Systems dominated by dry-deposited NH₃ downwind of intensive livestock farms or wet-deposited NH ₄ ⁺ and NO ₃ ^– in the upland regions of Britain resulted in approximately the same linear response. Emissions of NO and N₂O from these soils increased with both N deposition and KCl extractable NH ₄ ⁺ , but the relationship between NH ₄ ⁺ and N deposition (ln NH ₄ ⁺ = 0.62 ln N_deposition + 0.21, r ² = 0.33, n = 43) was more robust than the relationship between N deposition and soil NO and N₂O fluxes.     

Ozone Dry Deposition Velocities for Coastal Waters

Air-sea exchange rates for ozone were measured by the eddy correlation technique at a site on the north Norfolk coast in the UK. The average surface resistance to ozone uptake was found to be, r_s(O₃) = 1,000 ± 100 s m^-1. Micrometeorological measurements of trace gas fluxes to ocean surfaces are rare but a review of available measurements suggests that we can constrain sea water surface resistance for ozone to between 1,000 (Regener (1974), and this work) and 1,890 s m^-1 (Lenschow et al., 1982), yielding surface deposition velocities between 0.53 and 1.0 mm s^-1. These values are more than an order of magnitude greater than can be explained by laboratory determined mass accommodation coefficients for ozone to water. The importance of dry deposition with respect to process air-sea exchange models is highlighted. A trend in surface deposition velocity with wind speed was also observed supporting a surface chemical enhancement mechanism of ozone uptake which in turn is enhanced by near surface mixing processes.     

Development of Stream Water Chemistry during Spring Melt in a Northern Hardwood Forest

The role of snowmelt and subsurface hydrology in determiningthe chemistry of a small headwater stream in the TurkeyLakes Watershed (TLW) was evaluated for the spring meltperiods 1992 to 1996. Spring runoff is the dominanthydrological event at the TLW each year. Processesoccurring within the snowpack during snowmelt wereprincipally responsible for the above-ground changes inchemical fluxes relative to bulk deposition (the effect ofwinter throughfall was minimal). Large changes in chemicalfluxes occurred below ground. Organic matter decomposition,weathering, nitrification, and element cycling are some ofthe more important below-ground processes that operateduring the snow accumulation and ablation season and controlthe composition of the water ultimately appearing in thestream. Maximum stream discharge was accompanied byelevated concentrations of H⁺, NO₃ ^-, K⁺,NH₄ ⁺, DOC, Al and Mn, but reduced levels ofCa²⁺, Mg²⁺, SO₄ ^2- and SiO₂. Theconcentration-discharge relationships were consistent withwater movement through and above the forest floor duringpeak discharge, a flowpath facilitated by rapid infiltrationof meltwater and the existence of a relatively impermeablelayer in the mineral soil creating a perched water table. Averaged over the five periods of snow accumulation andablation, it was estimated that pre-melt stream flow, andwater routed through the forest floor and through the uppermineral soil contributed 9, 28 and 63%, respectively, ofthe discharge measured at the outlet of the catchment. Theforest floor contribution would be greater at peak dischargeand at higher elevations. An end-member mixing modelestimated concentrations of SO₄ ^2-, NO₃ ^-,Cl^-, Ca²⁺, Mg²⁺, Na⁺ and Al that werecomparable to average values measured in the stream. Othervariables (NH₄ ⁺, H⁺, K⁺ and DOC) wereover-estimated implying retention mechanisms operatingoutside the model assumptions.     

Quantifying dry NH3 deposition to an ombrotrophic bog from an automated NH3 field release system

Providing an accurate estimate of the dry component of N deposition to low N background, semi-natural habitats, such as bogs and upland moors dominated by Calluna vulgaris is difficult, but essential to relate nitrogen deposition to effects in these communities. To quantify the effects of NH₃ inputs to moorland vegetation growing on a bog at a field scale, a field release NH₃ fumigation system was established at Whim Moss (Scottish Borders) in 2002. Gaseous NH₃ from a line source was released along of a 60 m transect, when meteorological conditions (wind speed >2.5 m s^?1 and wind direction in the sector 180–215°) were met, thereby providing a profile of decreasing NH₃ concentration with distance from the source. In a complementary study, using a NH₃ flux chamber system, the relationships between NH₃ concentrations and cuticular resistances were quantified for a range of NH₃ concentrations and micrometeorological conditions for moorland vegetation. Cuticular resistances increased with NH₃ concentration from 11 s m^?1 at 3.0 μg m^?3 to 30 s m^?1 at 30 μg m^?3. The NH₃ concentration data and the concentration-dependent canopy resistance are used to calculate NH₃ deposition taking into account leaf surface wetness. The implications of using an NH₃ concentration-dependent cuticular resistance and the importance for refining critical loads are discussed.     

Chemistry of Selected High-Elevation Lakes in Seven National Parks in the Western United States

A chemical survey of 69 high-altitude lakes in seven national parks in the western United States was conducted during the fallof 1999; the lakes were previously sampled during the fall of 1985, as part of the Western Lake Survey. Lakes in parks in the Sierra/southern Cascades (Lassen Volcanic, Yosemite, Sequoia/Kings Canyon National Parks) and in the southern RockyMountains (Rocky Mountain National Park) were very dilute; medianspecific conductance ranged from 4.4 to 12.2 S cm^-1 andmedian alkalinity concentrations ranged from 32.2 to 72.9 eqL^-1. Specific conductances and alkalinity concentrations were substantially higher in lakes in the central and northernRocky Mountains parks (Grand Teton, Yellowstone, and GlacierNational Parks), probably due to the prevalence of more reactivebedrock types. Regional patterns in lake concentrations of NO₃ and SO₄ were similar to regional patterns in NO₃ and SO₄ concentrations in precipitation, suggestingthat the lakes are showing a response to atmospheric deposition.Concentrations of NO₃ were particularly high in Rocky Mountain National Park, where some ecosystems appear to be undergoing nitrogen saturation.     

Effects of Nitrogen Deposition on Bryophyte Species Composition of Calcareous Grasslands

Regular additions of NH₄NO₃ (35–140 kg N ha⁻¹ yr⁻¹) and (NH₄)₂SO₄ (140 kg N ha⁻¹ yr⁻¹) to a calcareous grassland in northern England over a period of 12 years have resulted in a decline in the frequency of the indigenous bryophyte species and the establishment of non-indigenous calcifuge species, with implications for the structure and composition of this calcareous bryophyte community. The lowest NH₄NO₃ additions of 35 kg N ha⁻¹ yr⁻¹ produced significant declines in frequency of Hypnum cupressiforme, Campylium chrysophyllum, and Calliergon cuspidatum. Significant reductions in frequency at higher NH₄NO₃ application rates were recorded for Pseudoscleropodium purum, Ctenidum molluscum, and Dicranum scoparium. The highest NH₄NO₃ and (NH₄)₂SO₄ additions provided conditions conducive for the establishment of two typical calcifuges – Polytrichum spp. and Campylopus introflexus, respectively. Substrate-surface pH measurements showed a dose-related reduction in pH with increasing NH₄NO₃ deposition rates of 1.6 pH units between the control and highest deposition rate, and a further significant fall in pH, of >1 pH unit, between the NH₄NO₃ and (NH₄)₂SO₄ treatments. These results suggest that indigenous bryophyte composition may be at risk from nitrogen deposition rates of 35 kg N ha⁻¹ yr⁻¹ or less. These effects are of particular concern for rare or endangered species of low frequency.     

An Automated Wet Deposition System to Compare the Effects of Reduced and Oxidised N on Ombrotrophic Bog Species: Practical Considerations

Critical N loads for ombrotrophic bogs, which often contain rare and N-sensitive plants (especially those in lower plant groups: lichens, mosses and liverworts), are based on very few experimental data from measured, low background N deposition areas. Additionally the relative effects of reduced versus oxidised N are largely unknown. This paper describes an automated field exposure system (30 km S. of Edinburgh, Scotland) for treating ombrotrophic bog vegetation with fine droplets of oxidised N (NaNO₃) and reduced N (NH₄Cl). Whim Moss exists in an area of low ambient N deposition (ca. 8 kg N ha^–1 y^–1), the sources and quantification of which are described. The wet N treatment system is run continuously, and is controlled/activated by wind speed and rainfall to provide a unique simulation of real world treatment patterns (no rain=no treatment). Simulated precipitation is supplied at ionic concentrations below4mMin rainwater collected on site. Treatments provide a replicated dose response to 16, 32 and 64 kg N ha^–1 y^–1 adjusted for ambient deposition (8 kg N ha^–1 y^–1). The 16 and 64 kg N ha^–1 y^–1 are duplicated with a P+K supplement. Baseline soil chemistry and foliar nutrient status was established for all 44 plots for Calluna vulgaris, Sphagnum capillifolium, Hypnum jutlandicum and Cladonia portentosa.     

Implications of Heterogeneous Chemistry of Nitric Acid for Nitrogen Deposition to Marine Ecosystems: Observations and Modeling

Size resolved particle composition and nitric acid (HNO₃)measurements from the ASEPS'98 experiment conducted in the BalticSea are used to provide observational evidence of substantialgas-particle transfer of oxidized nitrogen (N) compounds in themarine boundary layer. We then focus on the importance ofHNO₃ reactions on sea salt particles in determining spatio-temporal patterns of N dry deposition to marine ecosystems.Modelling results obtained assuming no kinetic or chemical limiton HNO₃ uptake and horizontally homogeneous conditions withnear-neutral stability, indicate that for wind speeds 3.5 – 10 ms^-1 transfer of HNO₃ to the particle phase to formparticle nitrate (NO₃ ^-) may decrease the N depositionvelocity by 50%. We extend this research using the CHEM-COASTmodel to demonstrate that, in a sulphur poor environment undermoderate wind speeds with HNO₃ concentrations representativeof those found in the marine boundary layer, inclusion ofheterogeneous reactions on sea spray significantly reducesmodelled NO₃ ^- deposition in the near coastal zone.     

Topographic Controls of Nitrogen,Sulfur, and Carbon Transport from a Tolerant Hardwood Hillslope

The lateral down-slope movement of water, NO₃ ^-, NH₄ ⁺, SO₄ ^2-, H⁺ and DOC through an ablation till was examined from 1987 to 1990 for a one hectaresoil catena on a steep hillslope with uniform forest cover at the Turkey Lakes Watershed (TLW), Ontario, Canada. Natural variation in the export of nutrients from the soil profile via soil water to Little Turkey Lake was assessed in relation to nutrient distribution in soil at different topographic positions.Subsurface throughflow exhibited dramatic differences in nutrientconcentrations and fluxes with slope position, largely reflectingthat of the soil horizons through which the water passed. GreaterNO₃ ^-, SO₄ ^2-, and DOC concentrations in subsurface water in the upper, well-drained hillslope were a reflection of enrichment by contact with more acidic, more developed podzols, and more favorable soil physical and biological conditions for NO₃ ^- retention in solution.Nutrient inputs to the lake were strongly influenced by increaseddown-slope transport of water, and increased SO₄ ^2-, N, and C retention in wetter, less-developed podzolic soils that characterize lower slope positions. An understanding of water movement and soil development variation withtopographic position was required to accurately estimate nutrient budgets for steep slopes at TLW.