Report for research conducted for the Park Research and Intensive Monitoring of Ecosystems Network (PRIMENet) EPA

Assistance Agreement CR826558-01-0 Title: Atmospheric Deposition in Mountainous Terrain: Scaling up to the Landscape 2003

PI: Kathleen C. Weathers, Institute of Ecosystem Studies, Box AB, Millbrook, NY Phone: (845) 677-5343; E-mail: weathersk@ecostudies.org Co-PIs and support: Gary M. Lovett, Institute of Ecosystem Studies, Box AB, Millbrook, NY Steven E. Lindberg, University of Tennessee, Knoxville, TN Samuel M. Simkin, Research Assistant II, Institute of Ecosystem Studies, Box AB, Millbrook, NY

Summary: Atmospheric deposition has long been recognized as an important source of pollutants and nutrients to ecosystems. The need for reliable estimates of total atmospheric deposition (wet+dry+cloud) is central, not only to air pollution effects researchers, but also for calculation of input-output budgets, and to decision-makers faced with the challenge of assessing various policy initiatives. Although atmospheric deposition continues to represent a critical environmental and scientific issue, estimates of total deposition still contain large uncertainties, particularly across heterogeneous landscapes such as montane regions. We developed an empirical modeling approach that characterizes total deposition as a function of landscape features such as vegetation type, elevation, topographic exposure, slope, and aspect. We measured indices of total deposition to the landscapes of Acadia (ACAD; 121 km2) and Great Smoky Mt. (GRSM; 2074 km2) National Parks. Using 300+ deposition point measurements, whose values ranged over an order of magnitude, and corresponding landscape attributes at each Park, we are constructing a general linear model relating the deposition index to the landscape variables. We are using a GIS database of digital elevation models and vegetation type, as well as wet and dry deposition data from the closest national network monitoring stations, to scale-up point measurements of total deposition fluxes and create park-wide maps of total deposition. Preliminary deposition maps show high spatial heterogeneity in the distribution of hotspots (highs) and coldspots (lows) of deposition across these Park landscapes. The EPA PRIMENet funding supported the data collection and sample analysis for this effort; current NPS funding will allow final statistical analysis and map creation.

Introduction: Atmospheric deposition is an important source of pollutants and nutrients to ecosystems (e.g., Likens et al. 1977, Weathers et al. 1986). Total deposition includes wet (rain and snow), dry (gases and particles) and cloud or fog (also rime ice) deposition. The National Atmospheric Deposition Program (NADP) provides good coverage of wet deposition at a national scale, and its continuous operation allows for detection of both spatial and temporal trends in wet deposition. However, there are not sufficient sites to look at small-scale (e.g., meters to 10s of kms) local variability. For example Great Smoky Mountains (GRSM) and Acadia National Parks (ANP) each have only one NADP site. Dry deposition is highly spatially variable (e.g., Lovett 1994), however, the national air chemistry monitoring stations (CASTNet) whose data are used in modeling dry deposition, are ~1/3 fewer than NADP, and station siting is limited, in part, by the expense of the infrastructure (e.g., towers). Cloud and fog chemistry monitoring has been limited to a few mountaintop sites in eastern North America (e.g., Mountain Acid Deposition Monitoring Program, MADPro; Driscoll et al. 2001, Andersen et al. 1999). Estimates of total deposition to landscapes are restricted to areas immediately adjacent to monitoring sites. Further, model assumptions for both dry and cloud deposition estimates make the resultant values for heterogeneous terrain highly uncertain (e.g., Weathers et al. 2000, CASTNet website: www.epa.gov/castnet/sites). In order to quantify total deposition to heterogeneous landscapes, it is necessary to capture local variability in fluxes. Previous work indicates that local variability in deposition rates can, in part, be controlled by such landscape features as aspect, elevation, vegetation type and the presence of gaps or edges (Weathers et al. 2000, Fig. 2). For example, as a result of orographic effects, cloud deposition, and possibly enhanced dry deposition (Johnson and Lindberg 1992, Weathers et al. 2000), atmospheric inputs to high elevations are greater than those to adjacent low elevation regions (e.g., Lovett and Kinsman 1990); coniferous forests are more effective scavengers of particles and gases than deciduous forests (Weathers et al. 2000), and edges and gaps have been show to have higher rates of atmospheric deposition relative to forest interiors (Weathers et al. 1992, 1995, 2001; Lindberg and Owens 1993). Variations in slope and aspect can influence deposition as well (Weathers et al. 2000). By measuring indices of deposition that include deposition via wet, dry and cloud processes, as well as local landscape features, this project was designed to produce an improved calculation of ecosystem inputs. These data and this analysis will permit scaling up from intensive measurement points (e.g., monitoring stations) to complete landscapes. This will lead to the identification of hot and cold spots of deposition across the landscape, and, ultimately, allow assessment of forest ecosystem function at the finer spatial scales required for many management decisions. Methods: Sites We focused our research on Acadia National Park (ACAD) in Maine (ACAD; 121 km2) and Great Smoky Mountains National Park (GRSM; 2074 km2) in Tennessee and North Carolina (Fig. 1). Both Parks have high rates of atmospheric deposition (Weathers et al. 1986, 1988, Johnson and Lindberg 1992, Ollinger et al. 1993), suspected deleterious effects of
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deposition on terrestrial and aquatic ecosystems, highly heterogeneous terrain, and local atmospheric monitoring programs (NADP and CASTNet, and for GRSM, MADPro). Indices of Deposition Direct measurement of atmospheric deposition rates via micrometeorological techniques (such as eddy correlation) or inferential methods (i.e., measurement of air concentrations and modeled deposition fluxes) is expensive and difficult to maintain. In addition, the assumptions of these methods are generally not applicable to heterogeneous canopies and complex topography (e.g., Lovett 1994). As a result, their use is generally limited to intensive monitoring sites, usually at low elevations, and they can give no indication of the range of variation of deposition across a complex landscape. For some ecological, management, and policy questions, the resolution and accuracy of these deposition data are insufficient. To be logistically and financially feasible, patterns of deposition in heterogeneous (mountainous) terrain must be determined using easy-to-measure indices that record spatial variation, are not subject to assumptions about homogeneity of terrain and canopy, and those indices must be related to measured deposition at an intensively monitored reference sites (e.g., NADP and CASTNet). We used two such indices of spatial patterns of deposition in this research: sulfate flux in throughfall (Lindberg and Garten 1988), and lead concentration in the surface soil (e.g., Weathers et al. 2000). While we had intended to use lead in the forest floor as our primary index at both sites, it was not possible to use this index at ACAD because of disturbance: a fire burned to mineral soil in about half the Park in 1947. Similarly, at GRSM, bear disturbance and logistical constraints made all but short-term throughfall collections problematic. Thus, sulfate flux in throughfall was the primary measurement made at ACAD, while lead concentration in the forest floor was the primary measurement at GRSM. These methods are explained in more detail below. Lead in surface soil Lead deposited to forests from the atmosphere is known to be retained by organic matter in the surface soil (e.g., Reiners et al. 1975, Friedland et al. 1984, Weathers et al. 1995, 2000). Once bound, Pb is relatively immobile, even under acidic conditions, and accumulates as deposition continues over many years (Smith and Siccama 1981). For example, at four southeastern U.S. watersheds, ranging from ~300-1000m elevation, the average annual export of Pb in streamflow represented only 1-2% of annual atmospheric deposition (Lindberg and Turner 1988). Thus lead concentration in the surface soil is a useful indicator of long-term average patterns of deposition across a landscape (Weathers et al. 1995, 2000). Because Pb in the atmosphere resides mainly on fine aerosols which can be dry deposited or scavenged by rain or cloud droplets (Graustein and Turekian 1989), Pb content in the surface soil is an index of total atmospheric deposition via the combination of wet, dry and cloud deposition pathways. The measurement of lead in surface soil is particularly useful for identifying historical patterns of deposition, indicative of depositional patterns that range from decades and centuries (Johnson et al. 1982).

Sampling design for lead In GRSM, we measured Pb concentration on 380 surface forest floor samples distributed randomly throughout the Parks. We used a stratified-random sampling design and selected sampling locations using a GIS. Due to logistical constraints, sampling locations were limited to the center swath of the park (Fig 2), and to areas not far from trails. In this way, locations were chosen that were 1) within the central swath of the park, 2) within 2 pixels (30-60 m) of trails, and 3) representative of the Park landscape (Table 1). We sampled forest floors that had been undisturbed for the last 50+ years. At each sampling location, GPS location was determined and stored and the characteristics of the site with respect to aspect, elevation, vegetation type, and slope were noted. Specific methods: At each sampling location, at least 8 (up to 16 where O horizon was thin) randomly located surface soil subsamples (Oe and Oa horizons) were collected with a 5.8 cm diameter soil corer. The subsamples were combined to yield one composite sample per location. Forest floor material was placed in Ziploc bags in the field and sent to the Institute of Ecosystem Studies (IES) laboratory for processing and analysis: Samples were dried at 60 C, weighed, sieved (8.0 mm mesh), ground in a Wiley Mill (number 20 mesh), ashed at 475 C for 4 hours, digested in 35% ultra-pure nitric acid, filtered with #42 ashless paper, brought to volume with deionized water and chemically analyzed for Pb using an Inductively Coupled Plasma spectrometer (ICP). Certified reference samples were included with each batch of samples processed. Sulfate in throughfall In areas of high S deposition, forest canopies exchange only small amounts of S between internal assimilated pools and external pools on the leaf surface. Sulfate is a particularly good tracer of deposition because it encompasses every major deposition process, almost equally, including dry, wet and cloud deposition. As a result, deposition of SO4= in throughfall (belowcanopy drip) has been shown in a variety of canopies to be a good measure of total S deposition to canopies (Lindberg and Garten 1988, Garten et al. 1988, Lindberg and Lovett 1992). In contrast, throughfall cannot be used to accurately measure atmospheric deposition of nitrogen (N) because NO3- and NH4+ are actively taken up by forest canopies (Lindberg et al. 1986, Lovett and Lindberg 1993). However, because N and S are deposited by similar processes (wet, gas and particle, and cloud deposition) there is a strong correlation between spatial patterns of S and N deposition across forested sites in North America (e.g., Lindberg and Lovett 1992, Lovett and Lindberg 1993, Ollinger et al. 1993), and along an elevation gradient (Miller et al. 1993). Thus, broad-scale geographic as well as elevational (e.g., Lovett et al. 1999) and forest edge studies (Weathers et al. 1992) indicate that SO4= deposition in throughfall is a good indicator of spatial patterns of atmospheric deposition of both S and N to the forest canopy. Sampling design for throughfall Because all throughfall samples needed to be collected on the same day and between precipitation events, we selected a set of 10 trail systems at ACAD that could all be visited in fewer than two days and that traversed elevation and vegetation gradients. We then used a GIS to randomly select locations along those trail systems. Analysis of the distribution of landscape

features throughout Mount Desert Island, the Acadia National Park, the trail buffer areas, and the points we sampled showed that those sites were representative of the larger areas (Table 2). Specific methods: Throughfall samples were collected in 8 (20.32 cm) polyethylene funnels with polywool plugs placed in the neck of each of the funnels to filter local organic debris. The water collected in funnels drained through a plastic column containing anion exchange resins (see Simkin et al., in press, for details of the samplers and method). In brief, the resin collector consisted of a funnel attached to an anion-exchange resin column (Fig. 4). As water passed through the column, sulfate, and other anions, were held on the column with >95% efficiency (Simkin et al., in press). The ionic bonds between anions in the sample and the positively charged exchange sites on the resin produce a more chemically stable sample than anions in solution, which allowed for monthly rather than event-based sampling. The ion exchange resin samples were retrieved from the field every 4-6 weeks during the summer of 2000. The resin columns were transported back to IES, extracted with a 1.0N KI solution and analyzed via ion-chromatography (IC) to determine the flux of anions over the period of resin column exposure. GIS Coverages Information for GIS datalayers we are using is as follows: ACAD Vegetation: coverage name: VEG79 raw datafile name: veg79.e00 (ArcInfo polygon coverage) projection: UTM zone 19 datum: NAD83 scale of source material: 1:9000 source material: interpreted from color infrared photography from August 1979 overflight originator: Acadia National Park (Karen Anderson) Elevation: coverage name: mdigrd2_fill1 raw datafile name: mdidtm.exe projection: UTM zone 19 datum: NAD27 (converted to NAD83 by Sam Simkin at IES) resolution: 30 m pixel originator: College of the Atlantic (Gordon Longsworth) from USGS 24k DEM GRSM Vegetation: coverage name: Great Smoky Mountains National Park Land Cover raw datafile name: gsmnp_lc.e00 (ArcInfo grid) projection: Albers Equal Area datum: NAD83
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resolution: 30 m pixel source material: Landsat TM satellite data citation: MacKenzie, M.D. 1993. The vegetation of Great Smoky Mountains National Park: Past, present, and future. Ph.D. Dissertation, The University of Tennessee, Knoxville, TN 154 p. originator: Southern Appalachian Man and Biosphere project (www.lib.utk.edu/samab) Elevation: coverage name: GSMNP 30 METER DEM raw datafile name: gsm_dem.e00 (ArcInfo grid) projection: Albers Equal Area datum: NAD83 resolution: 30 m pixel source material: 30 meter (1:24,000) digital elevation data from USGS EROS data center originator: Southern Appalachian Man and Biosphere project (www.lib.utk.edu/samab) Summary of Results (to the end of the EPA funding period): Much of the work that was completed with EPA funding included: (1) setting up and executing the data collection phase of the study--our data collection efforts were extensive, both in numbers of samples collected and in spatial extent of area covered; (2) gathering and validating GIS datalayers; (3) analysis of samples collected in the field; (4) setting up and maintaining the database. Thus, only preliminary results are reported here. National Park Service funding, which is now in place, will allow completion of the project. There are several highlights from the results obtained up to the end of the EPA funding period. We compared the distribution of landscape features throughout the Parks with the regions from which we collected samples, and were pleased to see that the sampling points provided an excellent representation of the larger areas (Tables 1 and 2). Therefore, our final deposition maps will cover the complete Park regions. Throughfall flux of S is consistently greater than bulk deposition, as shown by a comparison of co-located bulk and throughfall deposition collectors at low and high elevation sites at ACAD (Fig. 5). The additional S deposition is a result of a combination of dry and wet (cloud and other droplet capture) deposition. For these two locations, total S deposition is 2-fold and 3-fold greater under the canopy vs. in the open (low and high elevation locations, respectively). Overall, there was a ten-fold variation in indices of deposition within both GRSM and ACAD (Figs 6 and 7). Preliminary analysis suggests that deposition to conifer forests was consistently higher than to deciduous forests and that deposition was positively correlated with elevation; when combined, forest type and elevation explain most of the variance in deposition for both Parks. Preliminary deposition maps show hotspots of deposition in high-elevation conifer forests (Fig 8). Implications These early analyses suggest that landscape features, especially vegetation type (coniferous vs. deciduous vegetation) and elevation explain much of the variance in the deposition index data, thus relationships between GIS-available landscape features and total deposition can be established. In addition, hotspots (higher deposition) of deposition exist in the

landscape, often adjacent to cooler spots of deposition. Whether or not total deposition to the region of the Park is different using this spatially explicit model or deposition measured and modeled using data from the national networks, capturing the spatial variability in deposition may be important when evaluating links between deposition and biotic response, or when establishing watershed input-output budgets.

Presentations and Publications: Simkin, S.M., K.C. Weathers, G.M. Lovett, S.E. Lindberg, and D.N. Lewis. 2003. Atmospheric deposition hotspots within Acadia and Great Smoky Mountains National Parks. Spatial Odyssey 2003, December 1-5, 2003 Orlando, FL. National Park Service GIS meeting. Weathers, K.C., T.J. Butler, G.M. Lovett, V.R. Kelly and G.E. Likens. 2003. Emissions and Deposition of Atmospheric Pollutants: An update. NYSERDA meeting, October 2003 Lindberg, S.E. 2003. Dry Deposition of Mercury, Is It Real? Invited presentation at the SETAC Workshop on Mercury Monitoring and Assessment, Pensacola, FL. September 2003. Weathers, K.C., Simkin, S.M., G.M. Lovett, and S.E. Lindberg. 2003. Scaling-up point measurements of atmospheric deposition to mountainous landscapes: an empirical modeling approach. Cary Conference X, Millbrook, NY, April 2003. Weathers, K.C. 2002. Atmospheric Inputs and Ecological Function. A presentation for the Workshop on Ecological Thresholds, Woodrow Wilson Center, 4-5 November 2002. Simkin, S.M., K.C. Weathers, G.M. Lovett, S.E. Lindberg, D.N. Lewis and K. Schwarz. 2002. Scaling-up point measurements of atmospheric deposition to mountainous landscapes: an empirical modeling approach. Ecological Society of America Annual Meeting, Tucson, AZ. Weathers, K.C., G.M. Lovett, M.A. Arthur, S.M. Simkin. 2002. Watershed controls on streamwater nitrate concentrations, Catskill Mountains, NY. Ecological Society of America Annual Meeting, Tucson, AZ. Weathers, K.C., G.M. Lovett, S.E. Lindberg, and S.M. Simkin. 2001. Atmospheric Deposition to Heterogeneous Terrain: Scaling-Up to the Landscape. American Geophysical Union, Spring Meeting, Boston, MA. Weathers, K.C., G.M. Lovett, S.E. Lindberg, S.M. Simkin, D.N. Lewis, K. Schwarz and J. Beeler. 2000. Atmospheric Deposition to Complex Terrain: Scaling-Up to the Landscape. National Atmospheric Deposition Program Meeting, Saratoga Springs, NY. Weathers, K.C., G.M. Lovett, S.E. Lindberg, S.M. Simkin, D.N. Lewis and M.L. Chambers. 1999. Atmospheric deposition in mountainous terrain: Scaling up to the landscape. EOS, Transactions, American Geophysical Union, Volume 80 (No. 46), 16 November 1999. Page F390. Simkin, S.M., D.N. Lewis, K.C. Weathers, G.M. Lovett and K. Schwarz. In press, Determination of sulfate, nitrate and chloride in throughfall using ion-exchange resins. Water, Air and Soil Pollution. Weathers, K.C., S.M. Simkin, G.M. Lovett, S.E. Lindberg, In prep, Hotspots of Deposition: Vegetation and Elevation Controls on Total Atmospheric Deposition in Heterogeneous Landscapes. To be submitted to Ecosystems.

Acknowledgments: We are indebted to Kirsten Schwarz, Lala Chambers, Joe Beeler, and the staff at Acadia and Great Smoky Mountains National Parks for their many contributions to this work. Current funding to complete the project is via the National Park Service.

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References Cited: Anderson, J.B., R.E. Baumgardner, V.A. Mohnen, and J.J. Bowser. 1999. Cloud chemistry in the eastern United States, as sampled from three high-elevation sites along the Appalachian Mountains. Atmospheric Environment 33:5105-5114. Driscoll, C.T., G.B. Lawrence, A.J. Bulger, T.J. Butler, C.S. Cronan, C. Eagar, K.F. Lambert, G.E. Likens, J.L. Stoddard, and K.C. Weathers. 2001. Acidic deposition in the northeastern United States: Sources and inputs, ecosystem effects, and management strategies. Bioscience 51:180-198. Friedland, A.J., A.H. Johnson, and T.G. Siccama. 1984. Trace-metal content of the forest floor in the Green Mountains of Vermont - Spatial and temporal patterns. Water, Air, & Soil Pollution 21:161-170. Garten, C.T., E.A. Bondietta, and R.D. Lomax. 1988. Contribution of foliar leaching and dry deposition to sulfate in net throughfall below deciduous trees. Atmospheric Environment 22:1425-1432. Graustein, W.C., and K.K. Turekian. 1989. The effects of forests and topography on the deposition of sub-micrometer aerosols measured by lead-210 and cesium-137 in soils. Agricultural and Forest Meteorology 47:199-220. Johnson, A.H., T.G. Siccama, and A.J. Friedland. 1982. Spatial and temporal patterns of lead accumulation in the forest floor in the northeastern United States. Journal of Environmental Quality 11:577-580. Johnson, D.W., and S.E. Lindberg (eds.). 1992. Atmospheric Deposition and Nutrient Cycling in Forest Ecosystems. Springer-Verlag, New York. Likens, G.E., F.H. Bormann, R.S. Pierce, J.S. Eaton, and N.M. Johnson. 1977. Biogeochemistry of a Forested Ecosystem. Springer-Verlag, New York. Lindberg, S.E. and C.T. Garten. 1988. Sources of sulfur in forest canopy throughfall. Nature 336:148-151. Lindberg, S.E., G.M. Lovett, D.D. Richter, and D.W. Johnson. 1986. Atmospheric deposition and canopy interactions of major ions in a forest. Science 231:141-145. Lindberg, S.E. and G.M. Lovett 1992. Deposition and forest canopy interactions of airborne sulfur: results from the Integrated Forest Study. Atmospheric Environment 26A:14771492. Lindberg, S.E., and J.G. Owens. 1993. Throughfall studies of deposition to forest edges and gaps in montane ecosystems. Biogeochemistry 19:173-194.

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Lindberg, S.E. and R.R. Turner. 1988. Factors influencing atmospheric deposition, stream export, and landscape accumulation of trace-metals in forested watersheds. Water, Air, & Soil Pollution 39:123-156. Lovett, G.M. 1994. Atmospheric deposition of nutrients and pollutants to North America: An ecological perspective. Ecological Applications 4:629-650. Lovett, G.M., and J.D. Kinsman. 1990. Atmospheric pollutant deposition to high-elevation ecosystems. Atmospheric Environment 24A:2767-2786. Lovett, G.M. and S.E. Lindberg. 1993. Atmospheric deposition and canopy interactions of nitrogen in forests. Canadian Journal of Forest Research 23:1603-1616. Lovett, G.M., A.W. Thompson, J.B. Anderson, and J.J. Bowser. 1999. Elevational patterns of sulfur deposition at a site in the Catskill Mountains, New York. Atmospheric Environment 33:617-624. Miller, E.K., A.J. Friedland, E.A. Arons, V.A. Mohnen, J.J. Battles, J.A. Panek, J. Kadlecek, and A.H. Johnson. 1993. Atmospheric deposition to forests along an elevational gradient at Whiteface Mountain, NY, USA. Atmospheric Environment Part A- General Topics. 27:2121-2136. Ollinger, S.V., J.D. Aber, G.M. Lovett, S.E. Millham, R.G. Lathrop, and J.M. Ellis. 1993. A spatial model of atmospheric deposition for the northeastern United States. Ecological Applications 3:459-472. Reiners, W.A., R.H. Marks, and P.M. Vitousek. 1975. Heavy metals in subalpine and alpine soils of New Hampshire. Oikos 26:264-275. Simkin, S.M., D. N. Lewis, G.M. Lovett and K. Schwarz. In press, Determination of sulfate, nitrate and chloride in throughfall using ion-exchange resins. Water, Air and Soil Pollution. Smith, W.H. and T.G. Siccama. 1981. The Hubbard Brook Ecosystem Study - biogeochemistry of lead in the northern hardwood forest. Journal of Environmental Quality 10:323-332. Weathers, K.C., G.E. Likens, F.H. Bormann et al. 1986. A regional acidic cloud/fog event in the eastern United States. Nature 319:657-658. Weathers, K.C., G.E. Likens, F.H. Bormann et al. 1988. Cloud water chemistry from ten sites in North America. Environmental Science and Technology 22:1018-1026. Weathers, K.C., G.M. Lovett, and G.E. Likens. 1992. The influence of a forest edge on cloud deposition. Pages 1415-1423 in S. E. Schwarz and W. G. N. Slinn, editors. Precipitation Scavenging and Atmosphere-Surface Exchange- Volume 3. Hemisphere Publ. Co., Washington, D.C.

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Weathers, K. C., G. M. Lovett, and G. E. Likens. 1995. Cloud water deposition to a spruce forest edge. Atmospheric Environment 29:665-672. Weathers, K.C., G.M. Lovett, G.E. Likens, and R. Lathrop. 2000. The effect of landscape features on deposition to Hunter Mountain, Catskill Mountains, New York. Ecological Applications 10:528-540. Weathers, K.C., M.L. Cadenasso, and S.T.A. Pickett. 2001. Forest edges as nutrient and pollutant concentrators: Potential synergisms between fragmentation, forest canopies, and the atmosphere. Conservation Biology 15:1506-1514.

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Table 1: Comparison of percent land coverage in various landscape features thought to control deposition for Great Smoky Mountain National Park (Park), the region of the Park sampled for this project ("Sampled Swath"; see also Fig. 2), and the landscape features measured at sampling points (Sam. Loc.). Park Vegetation Type Percent (%) Conifer Decid Other Elevation (meters) 4 45 42 9 0.01 11 29 44 16 1 0.01 1 39 48 12 0.01 9 26 44 20 2 0.03 3 44 19 33 <1 8 23 34 27 8 0 13 82 5 11 87 3 34 66 0 Sampled Swath Sam. Loc.

0-500 501-1000 1001-1500 1501-2000 2001-2500 Slope (degrees) 0-10 11-20 21-30 31-40 41-50 51-70 Aspect (degrees) 0 - 90 91-180 181-270 271-360

23 25 25 26

26 24 25 25

19 18 34 29

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Table 2: Comparison of percent land coverage in various landscape features thought to control deposition for Mount Desert Island (MDI), Acadia National Park (Park; a subset of MDI) and the sampling locations for this project (Sam. Loc.; see also Fig 3). MDI Vegetation Type Conifer Decid Other Elevation (meters) 0-10 101-20 201-300 301-400 401-500 Slope (degrees) 0-10 11-20 21-30 31-40 41-50 51-70 Aspect (degrees) 0 - 90 91-180 181-270 271-360 27 22 26 22 28 22 28 22 18 37 22 23 70 22 6 2 <1 <1 50 33 13 4 <1 <1 34 40 19 6 <1 0 83 11 4 2 <1 61 25 9 4 <1 32 37 20 11 0 31 41 28 Percent (%) 30 53 18 60 40 <1 Park Sam. Loc.

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Figure 1: Location of study locations: Acadia National Park (ACAD), ME and Great Smoky Mountain National Park (GRSM), TN, NC (Weathers et al., in prep).

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Figure 2: Location of forest floor sampling at GRSM (Weathers et al., in prep).

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Figure 3: Location of throughfall collections sites at ACAD (Weathers et al., in prep).

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Figure 4: Throughfall resin collector used in this study (Simkin et al., in press).

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5 4 3 2 1 0
wet Monitoring site (160 m) throughfall

Figure 5: Sulfur fluxes (kg/ha/103-day period) at ACAD at low (160m) and high (413m) elevation locations for water collected in the open (bulk) and under the forest canopy (throughfall) (Weathers et al, in prep).

Sulfur kg/ha/103 day period

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Figure 6: Distribution of Pb concentration in forest floor samples throughout GRSM sampling area. Larger bubbles = higher concentrations (Weathers et al., in prep).

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Figure 7: Distribution of sulfate fluxes in throughfall throughout ACAD sampling area. Larger bubbles = higher concentrations (Weathers et al., in prep).

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Figure 8: Preliminary deposition map for GRSM showing "hot" (red) and "cooler" (green) spots of deposition. (Weathers et al., in prep.).

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