1 USDA Forest Service, Northeastern Research Station, Durham, NH, U.S.A.; 2 State University of

New York, College of Environmental Science and Forestry, Faculty of Environmental and Forest Biology, Syracuse, NY, U.S.A.; 3 USDA Forest Service, Northeastern Research Station, Parsons, WV, U.S.A.; 4 Appalachian Laboratory, University of Maryland Center for Environmental Science, Frostburg, MD, U.S.A.; 5 Syracuse University, Department of Civil and Environmental Engineering, Syracuse, NY, U.S.A.; 6 University of Maine, Senator George J. Mitchell Center for Environmental and Watershed Research, Orono, ME, U.S.A.; 7 Institute of Ecosystem Studies, Millbrook, New York, U.S.A.; 8 Pennsylvania State University, School of Forest Resources, 311 Forest Resources Lab, University Park, PA, U.S.A.; 9 US Geological Survey, Water Resources Division, Troy, NY, U.S.A.; 10 US Geological Survey, Water Resources Division, Montpelier, VT, U.S.A. (∗ author for correspondence, e-mail:, Fax: 603 868 7604) (Received 5 November 2002; accepted 27 July 2003) Abstract. Input-output budgets for dissolved inorganic nitrogen (DIN) are summarized for 24 small watersheds at 15 locations in the northeastern United States. The study watersheds are completely forested, free of recent physical disturbances, and span a geographical region bounded by West Virginia on the south and west, and Maine on the north and east. Total N budgets are not presented; however, fluxes of inorganic N in precipitation and streamwater dominate inputs and outputs of N at these watersheds. The range in inputs of DIN in wet-only precipitation from nearby National Atmospheric Deposition Program (NADP) sites was 2.7 to 8.1 kg N ha−1 yr−1 (mean = 6.4 kg N ha−1 yr−1 ; median = 7.0 kg N ha−1 yr−1 ). Outputs of DIN in streamwater ranged from 0.1 to 5.7 kg N ha−1 yr−1 (mean = 2.0 kg N ha−1 yr−1 ; median = 1.7 kg N ha−1 yr−1 ). Precipitation inputs of DIN exceeded outputs in streamwater at all watersheds, with net retention of DIN ranging from 1.2 to 7.3 kg N ha−1 yr−1 (mean = 4.4 kg N ha−1 yr−1 ; median = 4.6 kg N ha−1 yr−1 ). Outputs of DIN in streamwater were predominantly NO3 -N (mean = 89%; median = 94%). Wet deposition of DIN was not significantly related to DIN outputs in streamwater for these watersheds. Watershed characteristics such as hydrology, vegetation type, and land-use history affect DIN losses and may mask any relationship between inputs and outputs. Consequently, these factors need to be included in the development of indices and simulation models for predicting ‘nitrogen saturation’ and other ecological processes. Keywords: ammonium, input-output relationships, nitrate, nitrogen, nitrogen saturation, watersheds

1. Introduction In the Temperate Zone of North America, nitrogen (N) is generally considered to
Water, Air, and Soil Pollution 151: 373–396, 2004. © 2004 Kluwer Academic Publishers. Printed in the Netherlands.



be a growth-limiting nutrient for terrestrial ecosystems. However, during the past decade it has been proposed that elevated atmospheric N deposition may lead to N saturation, which has been defined as a condition that occurs when the availability of inorganic N is in excess of biotic demand (Aber et al., 1989; Ågren and Bosatta, 1988). If forest ecosystems were to reach this condition, several adverse effects would result, including nutrient imbalances in foliage, increased soil acidification and aluminum mobility, and excess NO− 3 in streams (Aber et al., 1989; Skeffington and Wilson, 1988; Stoddard, 1994). Consequently, elevated N may affect water quality, as well as the productivity and health of forests. In the northeastern United States, the concern over N saturation has primarily been in response to elevated N deposition associated with acidic deposition. Emissions of N have increased for more than 100 yr, largely as a result of fossil fuel combustion and greater reliance on N fertilizers (Galloway, 1998). Stricter − industrial emissions standards have reduced SO2 4 deposition, but N emissions, and hence N deposition, have remained high and relatively constant for the past several decades (Driscoll et al., 2001). Nitrogen amendment studies have shown that forest ecosystems in the northeastern United States have different responses to experimental N inputs (Aber et al., 1995; Adams et al., 1997; Christ et al., 1995; Gilliam et al., 1996; Kahl et al., 1993; Magill et al., 2000; McNulty et al., 1996; Mitchell et al., 2001a; Nadelhoffer et al., 1995). These differences depend on the initial N status of the site and the rate at which sites progress toward saturation (Aber et al., 1998). The heterogeneous nature of forest ecosystems, and the combined effects of factors (e.g. land-use history, forest cover, and hydrologic flow paths) have made it difficult to predict vulnerabilities to high N deposition within and across regions. Factors such as climate (Mitchell et al., 1996; Murdoch et al., 1998) and disturbance create further complexity, especially for temporal patterns of N loss in drainage waters (Aber et al., 2002). Small watersheds have long been recognized as a useful tool for investigating how ecosystems respond to changes caused by both natural and human perturbations (Bormann and Likens, 1979; Church, 1997; Likens and Bormann, 1995). Provided that loss to groundwater is negligible, watershed N accumulation or loss can be determined by subtracting outputs in streamflow from inputs from atmospheric deposition. This approach assumes that there is no source of N via mineral weathering and no significant gains or losses of N through gaseous exchange with the atmosphere. Mineralogical sources of N can contribute to N losses in some areas of the United States (Holloway and Dahlgren, 1999; Holloway et al., 1998), but are not an important source of N in watersheds of the northeastern United States. Nitrogen budgets may also be affected by N fixation and denitrification; however in our study watersheds, these gains or losses are thought to be negligible compared to fluxes through hydrologic pathways (Bormann et al., 1993; Bormann and Likens, 1979; Bowden et al., 1990; Bowden, 1986). Annual efflux of nitrogenous gases is minor (<0.1 to 1.5 kg N ha−1 yr−1 ) in relatively undisturbed, forest watersheds of the northeastern United States (Ashby et al., 1998; Bowden et al.,

the concern over N saturation has largely focused on the northeastern United States because this area receives some of the greatest amounts of N deposition in North America (Clarke et al. Several studies have compared streamwater concentrations of N (Hornbeck et al. The objectives of this analysis were to establish ranges for fluxes of inorganic N (NH4 -N and NO3 -N) in precipitation and streamwater and to determine if there are general spatial patterns in N retention across the region. Annual inorganic N budgets (NH4 -N and NO3 -N) were compiled for each watershed using stream and precipitation volume and chemistry data. and disturbance history were examined as possible controls on N cycling. A 1 June water . it is difficult to measure gaseous N flux at the small watershed scale because of the large spatial variability within watersheds (Bohlen et al. large-scale physical disturbance were considered. soil properties. data were compiled for 24 relatively small. Details about watershed characteristics and sampling procedures are given in Table I. Also. Results from individual watershed studies have provided data on N retention and loss in the northeastern United States. Past watershed N budget comparisons that have been conducted are limited to a small number of watersheds (Campbell et al.. Only small (<1000 ha). To examine N input-output budgets in this region. forest watersheds that were free of recent (at least 50 yr). Munger and Eisenreich. 2000... Stoddard. 1997. 2000) and problems associated with measurement methodology (Bowden et al. We identified 24 watersheds from 15 sites throughout the region that met the aforementioned criteria.. In North America. 2. there have been few attempts to synthesize these data to examine regional patterns. 2000). but these analyses do not include stream discharge data necessary to calculate fluxes. however. Furthermore.. Methods Watersheds were chosen based on size.NITROGEN INPUT-OUTPUT BUDGETS 375 1990. Forest cover. 1997. 1994). land-use. forest watersheds (Table I). Lovett et al. Data from the 11 most intensively studied watersheds were used to determine if there were general relationships between N retention and watershed characteristics. 2000) or target specific areas within the northeastern region of the United States (Goodale et al. These analyses will enable researchers to put results of individual watershed studies in a regional context and will provide a better understanding of how watersheds differ in their capacity to retain N. 1990).. These criteria eliminated local differences in N export related to deforested or developed land. However. 1986). These sites covered an area from 39 to 46◦ N latitude and 68 to 80◦ W longitude. hydrology. and sampling interval. it will improve our ability to predict N export and will help identify areas that may be sensitive to conditions of N saturation. only watersheds with sampling intervals of three weeks or less were chosen to ensure that seasonal patterns and higher flow events were adequately represented. 1983). Bowden..

68◦ 17 N. Cone Pond Hubbard Brook Hubbard Brook (NH02) Hubbard Brook (NH02) 10 On-site 250 250 Mt. (1990) Nelson (2002) 190 200 130 Bear Brook Weymouth Point Unnamed Tributary to Herrington Creek Bowl MD NH BE BW BU BL CPa USDA Forest Service Inst. 71◦ 03 N. CAMPBELL ET AL. 68◦ 06 N. 72◦ 10 N. (1990) Castro and Morgan (2000) – 57 – 44◦ 21 44◦ 20 44◦ 52 45◦ 56 39◦ 28 W W W W W N. 71◦ 24 N. 79◦ 41 N. L. of Maine Hornbeck et al. (1997) Edwards and Helvey (1991) 43◦ 56 43◦ 56 43◦ 56 43◦ 56 43◦ 54 43◦ 57 43◦ 55 44◦ 30 41◦ 59 44◦ 00 40◦ 44 43◦ 07 43◦ 07 43◦ 07 44◦ 29 39◦ 03 39◦ 03 39◦ 03 W W W W W W W W W W W W W W W W W W Underhill (VT99) Parsons (WV18) N. 73◦ 03 N. 71◦ 23 N. (ME09) – – 320 – 250 J. USDA Forest Service Hornbeck et al. 79◦ 41 63 On-site 400 510 Unnamed stream Cadillac Brook Hadlock Brook East Bear Brook Unnamed stream Unnamed tributary to Herrington Creek East Branch West Branch Upper Branch Lower Branch Cone Pond Inlet Watershed 6 Watershed 9 Unnamed stream Biscuit Brook Archer Creek Watershed 1 Watershed 4 Watershed 6 Watershed 8 Watershed 9 Watershed 4 Watershed 10 Watershed 13 a Intensively monitored site. Norton and Fernandez (1999) Hornbeck et al. (1990) Murdoch and Stoddard (1992) Mitchell et al. Agency collecting data Reference Latitude. of Maine USDA Forest Service Univ. (1997) Likens and Bormann (1995) Martin et al. 71◦ 44 N. 73◦ 02 N. 71◦ 45 N. 72◦ 32 W 127 127 On-site Acadia USDA Forest Service Univ. 68◦ 13 N. of Maryland Syracuse Univ. 69◦ 17 N. 71◦ 24 N. 71◦ 36 N. 79◦ 41 N. (2001b) Lynch and Corbett (1989) Campbell et al. (2000) Hubbard Brook (NH02) 26 ACC ACH EBBa WPT HCR Univ. 74◦ 13 N. . Park (ME98) – Greenville Stn. 74◦ 30 N. 77◦ 55 N. Ecosystem Studies Hornbeck et al. (2002) Hubbard Brook (NH02) Biscuit Brook (NY68) Huntington Wildlife (NY20) Leading Ridge (PA42) Bennington (VT01) 81 On-site On-site On-site 29 250 630 500 290 310 Sleepers River Fernow WV HB6a HB9a MTS BSBa HWa LRa LB4 LB6 LB8 SRa F4a F10a F13a US Geological Survey USDA Forest Service Hornbeck et al. b Calculated as the mean of the maximum and minimum elevation. longitude Name of NADP site (code) Distance to NADP site (km) Elevation of NADP site (m) Stream Site Cockaponset ME CT CT 41◦ 24 N. 71◦ 23 N.376 TABLE I Watershed characteristics and sampling regime State Abbrev. Success Biscuit Brook Huntington Leading Ridge Lye Brook NY PA VT USDA Forest Service US Geological Survey SUNY-ESF Pennsylvania State Univ. 73◦ 02 N. 79◦ 26 Stilwell Lake (NY51) West Point (NY99) Acadia Natl.

Fragiaquult Cone Pond Hubbard Brook BE BW BU BL CPa HB6a HB9a NITROGEN INPUT-OUTPUT BUDGETS Mt. Aeric Haplaquept Typic Dystrochrept. Water years start/stop Total years Sampling interval (wks. Epiaquod. Aeric Haplaquept Typic Haplorthod Typic Haplorthod Typic Haplorthod Aquic Haplorthod.TABLE I (continued) State Abbrev. flume V-notch weir Modeled V-notch weir H flume V-notch weir 271 394 15 31 33 13 68 18 990 135 123 840 860 760 750 570 670 790 500 880 640 380 Northern hardwoods Northern hardwoods Northern hardwoods Northern hardwoods Mixed northern hardwoods/spruce-fir Northern hardwoods Mixed northern hardwoods/spruce-fir Northern hardwoods Northern hardwoods Northern hardwoods Central hardwoods Lye Brook Sleepers River Fernow WV LB4 LB6 LB8 SRa F4a F10a F13a 1994–1995 1994–1995 1994–1995 1992–1993/1996–1997 1989–1990/1997–1998 1989–1990/1996–1997 1989–1990/1996–1997 1 1 1 5 9 8 8 2 2 2 1 1 1 1 Modeled Modeled Modeled V-notch weir V-notch weir H flume H flume 163 106 130 41 39 15 14 570 710 790 600 800 760 760 Mixed northern hardwoods/spruce-fir Mixed northern hardwoods/spruce-fir Mixed northern hardwoods/spruce-fir Northern hardwoods Central hardwoods Central hardwoods Central hardwoods Typic Haplorthod Typic Haplorthod Typic Haplorthod Typic Haplorthod Typic and Lithic Haplorthod Typic Haplorthod Typic Haplorthod Typic Fragiorthod Typic and Lithic Dystrochrept Typic Haplorthod Typic Dystrochrept. Haplorthod Typic Dystrochrept Typic Dystrochrept Typic Dystrochrept Typic Dystrochrept 377 . Success Biscuit Brook Huntington Leading Ridge NY PA VT MTS BSBa HWa LRa 1995–1996/1996–1997 1995–1996/1996–1997 1995–1996/1996–1997 1995–1996/1996–1997 1990–1991/1997–1998 1979–1980/1997–1998 1995–1996/1997–1998 1979–1980/1980–1981 1984–1985/1996–1997 1995–1996/1997–1998 1979–1980/1992–1993 2 2 2 2 8 19 3 2 13 3 14 2 2 2 2 1 1 1 1–3 1 1 1 Modeled Modeled Modeled Modeled V-notch weir V-notch weir.) Streamflow measurement Watershed area (ha) Elevationb (m) Vegetation Soil classification Site Cockaponset Acadia CT ME CT ACC ACH EBBa WPT HCR Bear Brook Weymouth Point Unnamed tributary to Herrington Creek Bowl MD NH 1980–1981/1984–1985 1999–2000 1999–2000 1989–1990/1998–1999 1980–1981/1986–1987 1996–1997 5 1 1 10 7 1 1–3 1–2 1–2 1 1–3 1 Modeled Stream contour Stream contour V-notch weir Modeled Stream contour 7 32 47 11 72 255 140 300 260 370 300 770 Central hardwoods Mixed northern hardwoods/spruce-fir Spruce-fir Northern hardwoods Spruce-fir Central hardwoods Typic Dystrochrept. Typic and Aquic Fragiudult Typic and Lithic Haplorthod Typic and Aquic Haplorthod Typic Humaquept. Hapludult.

differences in the concentrations of N in precipitation over a distance of less than 130 km are minor. 1995). These differences in distance and elevation.378 J. 2000).2 mg L−1 . Since N inputs are influenced more by the quantity of precipitation than by concentrations of N. 1990. NY) was discontinued in 1984. Hunt- . 2002.. six had NADP collectors located on-site (Table I). 2002). At Cockaponset. and aspect. Ollinger et al. indicate that concentrations of N in precipitation are not related to elevation.2 to 0. 1995). may affect estimates of N deposition (Weathers et al. CAMPBELL ET AL. A thorough description of NADP sampling and analytical procedures is available through the NADP program office (NADP. 1999). data from two NADP sites were used because the closest NADP site (Stilwell Lake. Miller et al. N concentrations in precipitation were based on data from the closest NADP site. However. 2002). However. precipitation measurements were obtained from the closest precipitation gage associated with each watershed. range in NO3 -N = 0. For watersheds that lacked on-site NADP collectors. (1995) found that in the northeastern United States. WY 1992–1993 is from 1 June 1992 through 31 May 1993) was used to calculate annual fluxes because this period usually provides the best correlation between annual precipitation and streamflow (Likens and Bormann. forest gaps.5 mg L−1 ) and our data.1 to 0. Lovett and Kinsman. we used weekly precipitation chemistry data from the National Atmospheric Deposition Program (NADP.g... NO3 -N was significantly related to longitude. year (e. Kahl et al. There are spatial trends in concentrations of N in precipitation across the region. The NADP collectors were located within 130 km of the watersheds and the difference in elevation between NADP collectors and the midpoint elevation of watersheds was <610 m (Table I).. Samples collected as part of the NADP program are sent to a central laboratory at the University of Illinois at Urbana-Champaign and are + analyzed for NO− 3 using an ion chromatograph and NH4 using a flow injection analyzer. For each NADP site. To determine watershed inputs. and both latitude and longitude were significant predictors of NH4 -N. At Acadia National Park. Wet deposition measurements at these sites are comparable to measurements from NADP sites since the equipment and methods used to collect data are nearly identical (Castro and Morgan. monthly input values were calculated by summing the product of weekly precipitation volume and chemical concentrations. we used long-term monthly means based on all the data available since the inception of the NADP program in WY 1979–1980. as well as differences in landscape features such as vegetation type. 1993. 2000. 2002) except at Bear Brook and the unnamed tributary to Herrington Creek where wet deposition data were collected independent of the NADP program. concentrations of N in precipitation are fairly uniform across these sites (range in NH4 -N = 0. Ollinger et al. Use of these NADP data assumes that N concentrations in precipitation at the closest NADP site were representative of N concentrations at corresponding watersheds. as well as data from other studies (Ito et al. In cases where there were insufficient data to characterize a monthly summary period (NADP. Of the 15 sites included in this study. L..

BROOK90 requires daily precipitation. they under-represent the total N atmospheric inputs. dry deposition data are measured on-site as part of the Clean Air Status and Trends Network (US Environmental Protection Agency. The model was run on a daily time step to predict streamflow expressed as mm day−1 . Federer and Lash. Several studies have shown that N deposited in cloud and fog water can be important at high elevation sites in the northeastern United States. For those water- . BROOK90 is a lumped-parameter model that can be used to estimate streamflow for small. such as the Huntington Forest (Lovett and Lindberg. For all other sites.. The only sites that did not have on-site precipitation collectors were Lye Brook and the Bowl. At each stream. At 14 of the watersheds. Streamwater outputs of N were calculated by multiplying mean concentrations by corresponding water fluxes. 1978) (Table I).1. and minimum and maximum air temperature input variables. At Fernow. VT and Tamworth. Dry deposition was not included in this analysis due to the paucity of data available. Ollinger et al. samples were collected at specified intervals (Table I) and were analyzed for NH4 -N and NO3 -N. Washington DC). forested watersheds.4. In a regional deposition model for the northeastern United States. and uncertainty associated with its measurement. Miller et al. such as those included in this study. NH. The model simulates vertical water movement at a single point. we used precipitation volume measured as part of the NADP program to calculate budgets. Cloud and fog water inputs were also not included in this analysis. However. The studies spanned different periods (1 to 19 yr) and typically used different protocols for sample collection and analysis (Table I). respectively) that were corrected for elevation using regression equations developed for each month of the year (Ollinger et al. and consequently works best for fairly uniform watersheds.6 kg N ha−1 yr−1 (6–36% of wet N deposition). 1993. (1995) determined that dry N deposition (measured as the sum of gaseous HNO3-N and particulate NO3 -N and NH4 -N) was approximately 20–46% of wet N deposition. Hubbard Brook and Lye Brook. 1993). Streamwater outputs were obtained from independent monitoring programs at each watershed.. or natural stream contours. 0. 1995). streamflow was measured using stage-height recorders and stream-channel controls including weirs. Mean annual dry N deposition at these sites was respectively 2. such as Whiteface Mountain in New York (∼6–7 kg N ha−1 yr−1 at 1000 m) (Lovett and Lindberg. N inputs in cloud and fog water are negligible. at lower elevation sites. For these sites. 1997. Since the N inputs reported in this study were based solely on wet deposition. and do not include dry deposition or deposition from fog and cloud water. and 2. precipitation measurements were obtained from closer rain gages operated independent of the NADP program. flumes. 1993) and Hubbard Brook (Weathers et al..NITROGEN INPUT-OUTPUT BUDGETS 379 ington and Leading Ridge. precipitation volume measurements were based on data from nearby (<10 km) National Weather Service (NWS) stations (Dorset. At the other 10 watersheds streamflow was estimated using the BROOK90 hydrological model (Federer. 1988).

this should not result in substantial errors in the export calculation of N since these solutes generally do not exhibit large responses to streamflow on an annual basis (Swistock et al. low flow period. evapotranspiration was calculated on a water year basis as the difference between precipitation inputs and stream discharge. Watersheds used in the detailed analysis were selected using more stringent criteria.5 kg N ha−1 yr−1 (Campbell et al. 1997). Measurements of solute export can be influenced by the frequency of data collection. Leading Ridge. sheds where streamflow was measured directly. Goodale et al. The dissolved organic fraction of N (DON) was not included in the N budgets for these watersheds. Fernow. Intermittent stream sampling generally characterizes low flow better than event flow because there is a greater likelihood that samples will be collected during the more common. 2000. which included: continuous streamflow measurement. 2000). and long-term records (>2 yr). Sleepers River). Although a significant fraction of N exports may be comprised of DON (Campbell et al. Cone Pond. particularly for elements that are well correlated with streamflow (Swistock et al. evapotranspiration was calculated by the model. We were not able to compare data for the same years at all sites because the collection periods varied in length and did not always coincide. Bear Brook. Of the 24 total watersheds included in the present study. a study of eight watersheds in Vermont and New Hampshire found that the net difference between DON inputs and outputs did not exceed 1. Budgets were developed by subtracting outputs from inputs. However. McHale et al. Export calculations differed according to the methods established at each watershed (Table I).. 2000). 2000. At some of the watersheds. Data collected before WY 1979–1980 were not used in this analysis because NADP data were not available before this time and because we wanted to analyze more recent patterns in N deposition and streamwater. L.. mean annual input and output values were calculated using all the data that were available since WY 1979–1980. .. CAMPBELL ET AL.380 J. and measured (rather than modeled) streamflow yield the best estimates of N output. weekly chemical sampling. Hubbard Brook. DON is measured in precipitation (independent of the NADP program) and more commonly in streamflow. At each watershed... For those sites where the hydrology was simulated with BROOK90. Huntington. event sampling. Data after 1997–1998 were not included because of the disturbance effects of a widespread ice storm that occurred in the region in January 1998. but the data have only been collected recently and analytical procedures vary among studies making comparisons difficult. 11 watersheds from 8 sites were selected for more detailed analyses (Biscuit Brook. 1997).. For NO3 -N and NH4 -N. greater sampling frequency.

Success to 1960 mm at the West Branch of the Bowl (Table II). WATER BUDGETS Annual average precipitation ranged from 900 mm at Mt. Precipi.1. 3.NITROGEN INPUT-OUTPUT BUDGETS 381 TABLE II Mean annual watershed hydrological budgets (mm ha−1 yr−1 ) for all the years available from WY 1979–1980 through WY 1997–1998. Annual average streamflow ranged from 290 mm at Weymouth Point to 1370 mm at the East Branch of the Bowl. Success Biscuit Brook Huntington Leading Ridge Lye Brook NY PA VT Sleepers River Fernow WV a Intensively monitored site.Stream.Evapotation flow transpiration flow transpiration (mm) (mm) (mm) (%) (%) CT ME CT ACC ACH EBBa WPT HCR BE BW BU BL CPa HB6a HB9a MTS BSBa HWa LRa LB4 LB6 LB8 SRa F4a F10a F13a 1350 1440 1440 1250 970 1430 1930 1960 1860 1860 1280 1420 1630 900 1520 1210 1050 1240 1330 1390 1320 1460 1450 1450 790 920 1080 920 290 940 1370 1360 1310 1300 670 900 1070 470 970 830 470 600 720 740 740 710 690 890 560 520 360 330 680 490 560 600 550 560 610 520 560 430 550 380 580 640 610 650 580 750 760 560 59 64 75 74 30 66 71 69 70 70 52 63 66 52 64 69 45 48 54 53 56 49 48 61 41 36 25 26 70 34 29 31 30 30 48 37 34 48 36 31 55 52 46 47 44 51 52 39 Cockaponset Acadia Bear Brook Weymouth Point Unnamed Tributary MD to Herrington Creek Bowl NH Cone Pond Hubbard Brook Mt.EvapoStream. and was . Evapotranspiration is calculated as precipitation minus streamflow. Results and Discussion 3. Streamflow and evapotranspiration are also expressed as a percentage of total precipitation Site State Abbrev.

such as Mt. the range was fairly wide even among watersheds with relatively long hydrological records (e.2 to 0.2 kg N ha−1 yr−1 ) were markedly lower.7 kg N ha−1 yr−1 (mean = 2. CAMPBELL ET AL.7 to 2.. L.5 mg L−1 and fluxes ranged from 1.4 kg N ha−1 yr−1 . Streamwater concentrations (<0. median = 7. streamwater concentrations (<0. Possible transformations that could cause low NH4 -N outputs include uptake by vegetation. there was a large range in streamwater NO3 -N exports. which had a net loss of 0. 3. Hubbard Brook Watershed 6. Annual contributions of NH4 N to the DIN retained in forest watersheds ranged from 0.1 mg L−1 ) and fluxes (<0. generation and processing of NO3 -N among watersheds. and adsorption on soil surfaces. D ISSOLVED INORGANIC N DIN (NH4 -N + NO3 -N) budgets show that at all watersheds. although in some cases the differences between inputs and outputs were relatively low. Biscuit Brook.8 mg L−1 ) and fluxes (<0. The range in DIN inputs was 2.2.1 to 5.7 kg N ha−1 yr−1 (26–92%). Outputs of DIN ranged from 0. it has been suggested that this watershed may be experiencing N saturation (Peterjohn et al. East Bear Brook.1 kg N ha−1 yr−1 ). and evapotranspiration may be partially due to the short sampling period at some sites. Concentrations of NH4 -N in precipitation ranged from 0. indicating large differences in the source.0 kg N ha−1 yr−1 .2 mg L−1 and fluxes ranged from 0.0 kg N ha−1 yr−1 ) except for Watershed 4 at the Fernow Experimental Forest. A MMONIUM Streamwater NH4 -N outputs were low and NH4 -N inputs in precipitation were consistently greater than streamwater outputs at all watersheds.0 kg N ha−1 yr−1 ). The relatively small outputs of NH4 -N indicate that nearly all the NH4 -N added in precipitation is being retained or transformed within these watersheds (Table III).1 to 5. 3. Annual average evapotranspiration ranged from 330 to 760 mm and was 25 to 70% of precipitation.g.9 to 2. In comparison.1 kg N ha−1 yr−1 (mean = 6. Success (0. The relatively large range in measurements of precipitation.4. streamflow. All other watersheds accumulated NO3 -N.7 kg N ha−1 yr−1 . precipitation inputs of DIN exceeded outputs resulting in a net DIN accumulation of 1. However unlike NH4 -N.8 kg N ha−1 yr−1 .3. median .5 kg N ha−1 yr−1 (Table III).3 kg N ha−1 yr−1 (Table III).1 to 5. 30 to 75% of precipitation.1 to 0.7 kg N ha−1 yr−1 ) were generally lower than concentrations and fluxes in precipitation. 1996).382 J. and Leading Ridge). However. microbial immobilization and nitrification. All watersheds retained NO3 -N on an annual basis (0.1 to 0.2 to 7. Since high leaching loss of NO3 -N is considered to be a sign that N inputs exceed the biological demand for N.. N ITRATE Concentrations of NO3 -N in precipitation ranged from 0. 3.8 to 5.7 to 8.

7 6.4 5.8 (26) 1.6 5.2 0.1 4.3 4.1 (41) 2.6 4.1 0. 383 .2 0.9 (67) 1.8 (56) 1.2 0.2 99 96 71 84 85 66 61 65 62 58 NITROGEN INPUT-OUTPUT BUDGETS Cockaponset Acadia Bear Brook Weymouth Point Unnamed Tributary to MD Herrington Creek Bowl NH a Intensively monitored site. Total percent DIN retention is calculated using the equation ([input-output]/input).1 0.4 5.0 3.2 2.5 2.1 5.3 (41) 0.1 1. NO3 -N. b Value is based on one water year (1992–1993).2 2.2 0.5 1.5 3.8 0.3 0.2 (49) 2.5 5.1 (46) 1.9 1.1 <0.0 (9) 2.8 7.4 (44) 1.6 0.8 2.6 (70) 2.4 2.6 0.9 (45) 5.3 (55) 6.4 6.8 4.3 (51) 2.5 4.9 4. and DIN (NH4 -N + NO3 -N) budgets (kg N ha−1 yr−1 ) for all the years available from WY 1979–1980 through WY 1997–1998.1 0.2 5.5 1.8 2.0 2.5 (54) 2.3 1.1 <0.2 0. Values in parentheses indicate respective percentage of NH4 -N and NO3 -N in DIN retained State Abbrev.0 (74) 2.TABLE III Mean annual watershed NH4 -N.0 2.7 2.9 2.1 0. Total N retention/loss is calculated as inputs minus outputs.7 2.2 2.3 0.8 4.5 1.4 (33) 1.8 3.2 2.0 3.9 3.0 (43) 2. Inputs Outputs Total N retention/loss Total DIN Site NH4 -N NO3 -N DIN NH4 -N NO3 -N DIN NH4 -N (%) NO3 -N (%) DIN retention (%) (kg N ha−1 yr−1 ) CT ME CT ACC ACH EBBa WPT HCR BE BW BU BL 2.3 3.4 7.1 1.2 7.3 0.2 2.5 4.2 1.2 3.7 (30) 2.3 2.1 0.6 7.1 0.6 (57) 3.9 (59) 1.

3 4.384 TABLE III (continued) State NH4 -N (kg N ha−1 yr−1 ) NO3 -N DIN NH4 -N NO3 -N DIN NH4 -N (%) NO3 -N (%) Abbrev.2 3.1 – 6.3 0.1 1.8 8.1 1.7 (33) 4.9 1.1 <0.4 4.8 2.2 1.8 (72) 3.1 4.7 1.7 (60) 2.3 (47) 2.1 0.1 6.1 <0.5 0.2 0.3 96 79 92 27 45 42 – 86 67 90 74 24 85 44 a Intensively monitored site.8 1.8 6.2 1.5 (76) 3.4 2.3 4.7 3.9 (61) 0.5 3.0 2.7 4.5 (40) 2.0 1.4 7.1 2.8 4.8 6.5 7.4 1.2 4.4 3.8 (24) 5.0 2.2 0.7 5.3 5.1 2.3 4.7 1.6 3.5 (28) 1.3 4. .5 3.7 1.1 <0.6 (50) 4.1 (65) 4. CAMPBELL ET AL.2 (69) 0.7 3.7 (35) 1.1 5.0 5.1 <0. Inputs Outputs Total N retention/loss DIN Total DIN retention (%) Site Cone Pond Hubbard Brook J.1 0.6 4.6 0.0 5.8 2.5 2.6 (50) 2.0 3. Success Biscuit Brook Huntington Leading Ridge Lye Brook NY PA VT Sleepers River Fernow WV CPa HB6a HB9a MTS BSBa HWa LRa LB4 LB6 LB8 SRa F4a F10a F13a 1.3 (70) 1.1 (92) 2.5 7.7 (37) 2.2 5.1 1.1 7.4 2.9 (31) 1. Mt.3 2.1 <0.2 0.5 0.2 4.6 2.5 6.7 1.1 0.2 7.1 0.1 6.1 (8) 1.0 (30) 0.6 (53) –0.2 7.6 5.4 (67) – 2.5 (39) 2.9 – 1. b Value is based on one water year (1992–1993).7 <0.1 4.2 – <0.0 7.6 7.4 5.0 5.1 0.5 2.6 (63) 2.1b 0.7 2.5 2.4 3. L.0 2.5 2.2 5.7 5.

with NO3 -N constituting a greater proportion of DIN outputs compared to NH4 -N at most watersheds. the lowest wet N inputs were found at the inland sites in Maine (East Bear Brook and Weymouth Point). 2002). In the northeastern United States. retained much less of the annual wet N input (24 and 27% respectively). In our study. nearly all the wet N deposition was retained within the watershed (99.g. which are at the extreme northeast portion of the study region. differences in atmospheric concentrations of N may be small or local factors that affect precipitation volume (e. In some cases. A portion of the variability in stream N outputs may also be attributed to differences in sampling procedures as well as to the duration of each study (Table I). Other watersheds. 3. Fluxes were highly variable even among adjacent watersheds that had similar characteristics and N loading. R EGIONAL PATTERNS The watersheds we examined occur along a gradient of atmospheric N deposition. New York. and that NH4 -N is lower in precipitation and near zero in streamwater. Wet deposition of N at the other watersheds did not exhibit distinct spatial patterns (e. gradients of increasing N deposition toward emission sources in the midwestern United States). The large range in stream N exports. Sleepers River) with more intensive long-term monitoring programs were investigated beyond the analysis of the larger . Cadillac Brook at Acadia.g. the greatest N deposition occurs in Pennsylvania.NITROGEN INPUT-OUTPUT BUDGETS 385 = 1. western Maryland and northern West Virginia (NADP. 3. and Weymouth Point. Cone Pond. The only watersheds where NH4 N outputs were greater than or equal to NO3 -N outputs were Cockaponset. indicates differences in N cycling within watersheds. compared to the more narrow range in precipitation inputs. such as Cockaponset. median = 71%). Hubbard Brook. These data indicate that NO3 -N is typically the dominant form of inorganic N in both precipitation and streamwater. There were no apparent regional patterns in streamwater exports of N. Cone Pond. Percent N watershed retention ranged from 24 to almost 100% (mean = 69%. Huntington. A NALYSIS OF MORE INTENSIVELY MONITORED SITES To address some concerns that may be associated with sampling at several sites. Leading Ridge. At these watersheds. eleven watersheds (located at East Bear Brook. These sites have lower N concentrations and receive less rainfall (due to lower elevation). 96.5. and Cadillac Brook at Acadia. Fernow. Biscuit Brook.7 kg N ha−1 yr−1 ). Results for streamwater were similar.6. such as Watershed 4 at the Fernow Experimental Forest and Mt Success. and consequently have lower N inputs. respectively). and 96%. Use of NADP data eliminated potential problems because of site differences in chemical techniques and the calculation of wet N inputs. NO3 N constituted a greater proportion of DIN inputs compared to NH4 -N. elevation) may confound regional spatial relationships. At all watersheds. Cone Pond. so spatial patterns in N retention among watersheds of the region were assessed.

3.49.7. r2 = 0. There was a significant relationship between mean annual streamflow and precipitation (streamflow (mm) = 0. The large range in precipitation among sites partially arises from the range in watershed elevation. P < 0. Table III). Figure 1. Since hydrological values are used to calculate fluxes.25. there was still a large range in percent DIN retention (24 to 96%).386 J. to 880 m at Biscuit Brook.02) at the intensively monitored sites indicating that streamflow is primarily affected by the amount of precipitation falling on a watershed rather than other factors such as differences in flow paths and vegetation.72 × precipitation (mm) – 181. For these watersheds. There was .5 kg N ha−1 yr−1 and stream outputs ranged from 0. For these intensively monitored sites. wet DIN inputs in precipitation ranged from 3. FACTORS AFFECTING N RETENTION One of the main objectives of our analysis was to examine factors that affect N retention in forest ecosystems. CAMPBELL ET AL.2 to 5.8 to 7.7 kg N ha−1 yr−1 (Figure 1. The mid-point elevation of the intensively monitored watersheds (calculated as the mean of the maximum and minimum watershed elevation) ranged from 370 m at East Bear Brook. Output data for Leading Ridge (LR) do not include NH4 -N values because NH4 -N was not measured in streamwater at this site. data set. L. Inputs of DIN in wet-only precipitation and outputs of DIN in streamwater (kg N ha−1 yr−1 ) at the more intensively monitored study watersheds. factors that affect precipitation or streamflow volume can also affect inputs and outputs of N.

8. at European watersheds with N inputs of less than 10 kg N ha−1 yr−1 .39.8.005 × elevation (m) + 3.. 2001). Influence of Hydrology Hydrologic flow paths can be a major factor influencing N retention and temporal patterns of stream N loss in forest watersheds (Mitchell. 1988. P < 0. In a synthesis of N watershed budgets in Europe. 3.69. P < 0. 1987) and high flow events (Wigington et al..17.84 × elevation (m) + 816. 3.001). r2 = 0. The relationship between wet DIN deposition and elevation was also significant (N inputs (kg N ha−1 yr−1 ) = 0.74. r2 = 0. Site characteristics. P < 0. Lovett and Kinsman. FACTORS CONTROLLING N RETENTION Complex processes that occur within watersheds regulate N export. Dise and Wright (1995) found that bulk inputs of inorganic N in precipitation were the most important predictor of N exports in streamwater of 41 variables examined (N outputs (kg N ha−1 yr−1 ) = 0..1 kg N ha−1 yr−1 ) of the watersheds in our study. Watersheds with thin or porous soils and high infiltration rates have less capacity to retain N (Lajtha et al. forest cover. largely influence these interactions and further complicate assessment of the relationship between N inputs and outputs.1. 1990). Rascher et al. However. 1987.43. presumably because deposition of N is much lower in the northeastern United States compared to Europe. 1995). There was not a significant relationship between wet DIN inputs and stream outputs for the intensively monitored watersheds in our study.. nearly all the N was retained and most of the significant leaching was found at watersheds receiving inputs greater than 25 kg N ha−1 yr−1 . Similarly. and land-use.48 × N inputs (kg N ha−1 yr−1 ) – 2. such as hydrology. Differences between bulk deposition and wet deposition are not nearly enough to account for this discrepancy and estimates of total N deposition in the northeastern United States (wet and dry) are thought to be less than 12 kg N ha−1 yr−1 (Ollinger et al. numerous studies have shown that NO− 3 rapidly leaches through soils to streams during snowmelt runoff (Galloway et al. 1996). The threshold of 25 kg N ha−1 yr−1 exceeds even the highest wet N inputs (8. .52.001) showing that high-elevation watersheds typically received the greatest amount of precipitation. The relationship between discharge and N export is typically stronger during the dormant season when biotic retention of N is lower. 1995)..NITROGEN INPUT-OUTPUT BUDGETS 387 a significant relationship between precipitation and elevation at these watersheds (precipitation (mm) = 0. At some of the European sites bulk N inputs exceeded 60 kg N ha−1 yr−1 . This relationship is primarily due to orographic effects and is consistent with similar studies in the northeastern United States (Dingman et al.04) indicating that the higher elevation sites included in this study also receive higher wet N deposition. r2 = 0..

coniferous species also have a much lower demand for N. Lovett et al. Since NO3 -N in deep groundwater is affected by reduced biotic activity. Furthermore.. while during the summer this relationship was not evident. and relatively high N stream losses during the growing season. Lovett et al. This lack of a relationship between forest cover and DIN loss provides further evidence of multiple controls on N retention. which under conditions of high N deposition could contribute to greater leaching losses. concentrations of NO3 -N remain relatively high throughout the growing season. They concluded that hydrologic differences are probably not driving differences in NO3 -N concentrations among watersheds. and hypothesized that among-watershed differences in tree species composition and historical land-use patterns described in the following sections are more likely to explain spatial patterns of N export and retention in the Catskill Mountains. (1998) suggested that high streamwater NO3 -N concentrations that occur throughout the growing season are the result of a deep groundwater source of NO3 -N. L. At Biscuit Brook.388 J.2. but no clear relationship was evident (Figure 2). This conclusion contrasts to the findings of Creed and Band (1998). Burns et al. working within a series of watersheds in Canada with more uniform vegetation than the Catskills. CAMPBELL ET AL. McNulty et al.8. Groundwater in this watershed is recharged with NO3 -N during the fall and early spring. (2000) found a poor relationship between NO3 -N concentrations and physical features of Catskill watersheds that might be expected to affect hydrologic residence times. there was only a strong relationship between NO3 -N and Ca2+ at high NO3 -N streams during the winter. 1991) and coniferous species typically have higher C:N ratios than deciduous species due to the lower N concentration of litter. Murdoch and Stoddard (1992) observed increases in NO− 3 concentrations with increasing discharge throughout most of the year. This pattern suggests that the relationship between NO3 -N and Ca2+ is due to NO3 -N induced leaching of Ca2+ and is not indicative of a groundwater source of NO3 -N. a relationship between Ca2+ and NO3 -N would be expected since Ca2+ concentrations in groundwater are high due to greater contact with less-weathered bedrock and deep till. The importance of forest cover was evaluated with respect to NH4 -N and NO3 -N outputs. Several hypotheses have been proposed to explain the high exports of NO3 -N (4. This groundwater provides NO3 -N to surface waters during base flow in summer. They suggested the importance of topography and hydrological factors in controlling surface water NO3 -N concentrations. 1998.0 kg N ha−1 yr−1 ) at Biscuit Brook. Higher C:N ratios generally result in higher N immobilization and hence low N leaching at coniferous sites. Soil C:N ratios have been shown to be good predictors of DIN export in drainage water (Gundersen et al. However. (2000) reasoned that if groundwater sources of NO3 -N drive streamwater NO3 -N concentrations. However.. Influence of Vegetation The effect of forest cover on N retention may be due to differences in N uptake and litter quality. 3. .

little seasonal variability in streamwater NO3 -N concentrations. and deciduous forest cover types for each watershed. For the Fernow watersheds investigated in our study... An important factor . size.NITROGEN INPUT-OUTPUT BUDGETS 389 Figure 2. and all samples are collected and analyzed using the same methods. long-term increases in streamwater concentrations of NO3 -N and base cations. (1998) examined N2 O production measured at plots within the boundary of Watershed 4 to evaluate factors that influence susceptibility to N saturation. Despite a poor overall relationship between forest cover and N retention among our study watersheds. air temperature. and is possibly the best case of an N-saturated site in North America (Peterjohn et al. 1996). parent material. Differences in N2 O production among plots did not appear to be associated with differences in soil temperature. 1996). 2000). relatively high NO3 -N concentrations in soil solutions. soils. Peterjohn et al. A principal mechanism driving differences in stream N losses at the Fernow Experimental Forest may be related to vegetation. other studies have shown that vegetation plays an important role in regulating N losses (Lovett and Rueth. elevation. N deposition). Several symptoms of N saturation have been identified at the Fernow Experimental Forest including high rates of net nitrification. mixed. The three Fernow watersheds have similar climatic and watershed characteristics (e.. Watershed 10 had relatively low NO3 -N exports and retained 85% of wet DIN deposition. Watershed 13 had the second highest NO3 -N outputs and retained less than half of wet DIN inputs. Streamwater DIN outputs (kg N ha−1 yr−1 ) on a gradient from dominant coniferous to dominant deciduous forest cover. In contrast. and low retention of inorganic NO3 -N compared to other forest watersheds (Peterjohn et al. Values in parentheses indicate respective percentage of coniferous.g. The Fernow Experimental Forest is showing signs of N saturation. Data for Leading Ridge (LR) do not include NH4 -N values because NH4 -N was not measured in streamwater at this site. hydrology. Watershed 4 retained only 24% of wet DIN deposition and was the only watershed where mean annual stream NO3 -N outputs exceeded inputs. The three watersheds of the Fernow Experimental Forest provide an example of how vegetation may influence N retention. water filled soil pore space. or soil pH. Magill et al. 1999.

2000. however.. which could contribute to the high NO3 -N losses. agriculture and grazing. a comparison of samples collected during 1973–1974 and 1994–1997 indicated that streamwater NO− 3 concentrations have significantly decreased over this 20 yr period (Martin et al. 1984.. This stand now appears to be deteriorating rapidly as a result of wind damage. streamwater NO− 3 concentrations tend to be elevated throughout the year. 2000). including the growing season. plots with low N2 O production were characterized by a greater proportion of species associated with lower rates of soil nitrification (e. It is also possible that the herbaceous layer may influence N retention among Fernow Watersheds. influencing N2 O production in Watershed 4 appears to be differences in NO− 3 availability associated with tree species composition (Peterjohn et al.g. In contrast.g. Plots with the highest N2 O production were dominated by tree species characterized by low leaf lignin and high soil nitrification rates (e. Fernow Watershed 4 had a relatively high proportion of old-growth beech and sugar maple (some trees may reach 300 yr old). . approximately 85% of the watershed was heavily burned around 1820 as indicated by the presence of soil charcoal (Buso et al. may strongly affect N retention. 1999). sugar maple (Acer saccharum)). as well as those of other studies in the northeastern United States (Lewis and Likens.390 J. Only a small proportion of the Cone Pond watershed has been harvested. red oak (Quercus rubra) and American beech (Fagus grandifolia)). indicating an excess of N (Martin et al. These speciesrelated differences in N retention are consistent with the results for the Catskill streams described in the previous section. The successional status of vegetation may be important in regulating N losses and it has been suggested that aggrading forests may have lower NO− 3 losses because they are thought to have a higher demand for N (Vitousek and Reiners. 3. Stream export of N from the Bowl may also be affected by the old-growth status of the forest. 1997). 1975). L. While N retention at the Bowl (58–65%) was not excessively low compared to some of the other watersheds we investigated. (2001) found that plots within Watershed 4 with low soil water NO− 3 concentrations were found in areas where lowbush blueberry (Vaccinium vacillans) was common.. Hornbeck and Lawrence. The Cone Pond watershed is predominantly coniferous and is comprised of unevenaged trees. Lowbush blueberry has been shown to acidify the soil. other land disturbances such as fires.8. 2000). A good example of the influence of fire on N retention is at the Cone Pond watershed. 1999).. Despite this observation. Lovett and Rueth. some of which are over 250 yr old. which strongly retained N on an annual basis (96% DIN retention) and had outputs of NO3 -N that were among the lowest of the streams included in our study. CAMPBELL ET AL. thereby reducing soil N mineralization and nitrification.3. Influence of Fire/Land-use While forest successional status and logging history are important. presumably due to higher rates of N cycling associated with more rapid litter decomposition. Gilliam et al.

However. The Cockaponset watershed was also used as pastureland prior to re-growth of the present forest. These findings suggest that although the fire at Cone Pond occurred over 180 yr ago. this pulsed release of DIN to streams is generally short-lived. and greater DIN runoff due to reduced evapotranspiration (Tiedemann et al. High streamwater exports of N may be an indication that some watersheds are approaching a condition of N saturation. Currently. there has been a lasting effect on C and N pools resulting in low NO3 -N exports. The initial loss of C and N was followed by re-growth of red spruce (Picea rubens) and balsam fir (Abies balsamea) vegetation.. soil C:N ratios in the burned areas of the watershed are high (>30:1) compared to unburned areas (17:1) (Hornbeck and Lawrence.1 kg N ha−1 yr−1 ) and high (nearly 100%) DIN retention. The lower portion of the watershed was used as pastureland until the late 1890’s. 1992. Data from Europe show that significant N leaching occurs when inputs exceed 25 kg N ha−1 yr−1 . 1978. Schindler et al. thereby reducing soil C and N content. whereas other watersheds had outputs that were closer to wet N inputs. 2002). However. 1976)... whereas the neighboring Cadillac Brook watershed was largely burned by wildfire in 1947. Some watersheds retained nearly all of the wet N deposited on an annual basis. the DIN outputs are much lower at Cadillac Brook (0. All of these land-use practices may reduce the soil C and N stores resulting in low stream NO3 -N losses (<0. as DIN is rapidly taken up by aggrading vegetation (Bayley et al. 1980). 1973. 1997). Conclusions Export of DIN in streamwater was less than wet-only DIN input at all of the watersheds included in our study. streamwater DIN export may increase as a result of higher nitrification associated with warmer soil temperatures.NITROGEN INPUT-OUTPUT BUDGETS 391 In the few years following fire. the large differences in percent N retention indicate that watersheds vary widely in their ability to retain N. causing a reduction in NO3 -N leaching.3 kg N ha−1 yr−1 ) (Nelson. 4. Brown et al. High soil C:N ratios and poor litter quality may limit nitrification and NO3 N production. Data from the paired watershed study at Acadia reinforces our interpretation of the influence of fire on N retention. Although many of the characteristics between the two Acadia watersheds are similar. and was severely burned during this period.. Bormann and Likens. 1979. the upper portion of the watershed was clear-cut in the mid to late 1800’s for charcoal production. Long-term effects of severe fires typically reduce soil C and N storage by volatilization of C and N compounds.2 kg N ha−1 yr−1 ) compared to Hadlock Brook (1. At Leading Ridge. In contrast. The fire at Cone Pond is thought to have been sufficiently severe to remove most of the soil organic matter. differences in N retention among watersheds in . The Hadlock Brook watershed at Acadia has been left largely undisturbed. Wright. which has poor quality litter with a high lignin:N ratio.

. However. Aber. R. but is still poorly understood on a regional scale. McDowell. for the Fernow Experimental Forest. Downs.392 J.. Rustad. Magill. D. and US Geological Survey. disturbance. and Mary Flagler Cary Charitable Trust. and dry N deposition. BioScience 48. 921–934. Northeastern Research Station. geology. J. and Melillo. National Science Foundation... Water. and Soil Pollut. J. many unanswered questions still remain. Berntson. denitrification. Environmental Protection Agency and the USDA Forest Service. Nadelhoffer... J. K. 85. Air. The role of some of these factors has been addressed at the plot or watershed level. J. References Aber. for the Unnamed Tributary to Herrington Creek.. M. These controls affect C and N pools within watersheds and ultimately influence the release of N to streams.. for Hubbard Brook. We thank Tom Luther for geographic analysis. the Environmental Protection Agency. The Pennsylvania State University Agricultural Experiment Station through funds received from the McIntire-Stennis Cooperative Forestry Research Program. K. L. Boone. Magill.. J. S. McNulty. J. McNulty. Rather these differences appear to be the result of a complex combination of factors involving vegetation.: 1998.. G.. the Maryland Department of Natural Resources. Steudler. A. An earlier version of this manuscript was improved by comments from Russell Briggs. 1665–1670. for Leading Ridge. G. National Science Foundation. ‘Forest biogeochemistry and primary production altered by nitrogen saturation’. our study were not directly related to N loading. and National Park Service. vegetation influences. W. and soils. W. data from watershed studies have provided advances in our understanding of N cycling in forested watersheds. CAMPBELL ET AL. Aber. D. Acknowledgements This research was funded by the Northeastern Ecosystem Research Cooperative. D... The Andrew W. ‘Nitrogen saturation in temperate forest ecosystems’. A. L.: 1989. The results presented here suggest that regional analyses combined with specific case studies are needed to evaluate the spatial and temporal patterns of N solute loss in surface waters of the northeastern United States. 378–386. and Fernandez. BioScience 39. Kamakea. for Bear Brook.: 1995. the Environmental Protection Agency. I. P.. M. K. M.. R. and Hallett. such as those related to the importance of hydrology. Mellon Foundation. N fixation. In recent years. Currie. landuse. ‘Nitrogen saturation in northern forest ecosystems’. US Geological Survey. Nadelhoffer. Financial support for long-term monitoring at individual research sites was provided by the following institutions: for Acadia. Nadelhoffer. S. .

U. B. Wang. Likens. ‘Effect of groundwater springs on NO− 3 concentrations during summer in Catskill Mountain streams’. Can. E.. B. W. M. alder. G. S. Biogeochemistry 2.: 2002. W. J. C. 34. 79–91. Buso.: 2000. T. and Morgan. E. E. Biochem. E. J. A. R. 234–248. 30. L.A. Campbell.. J. M. 1987–1996. New York.. E. G.. Ecology 82.. C. Bormann. and Band. E.: 2000. and Murdoch. Water Resour.. ‘Export of nitrogen from catchments within a temperate forest: Evidence for a unifying mechanism regulated by variable source area dynamics’. West Virginia’. For. L... W.S.. Steudler. ‘Hydrochemistry of forested catchments’. Bormann. 853–864. C. ‘Dry deposition calculations for the clean air status trends network’. ‘Rapid N2 fixation in pines. and Marston. R. and Melillo. P. 13997–14005. J.. B. D.: 1992. Water Resour. I. and Soil Pollut. J. Eagar. B. Environ. Church. B. W.. S. ‘Controls on dentrification in riparian soils in headwater catchments of a hardwood forest in the Catskill Mountains. G. M. Res. H. F. C. McDowell. and Stainton. 123–142. Creed.. G. and Driscoll. Driscoll. and Siccama. W. Res. W. R. New Hampshire Water Resources Research Center.: 1998. J. 583–598. Air. Brown. B.. A.. Christ. Martin. L. T. R. Res. Driscoll. and Hornbeck. ‘Nitrogen saturation of terrestrial ecosystems’. T. 3667–3678. Castro. Manage. R. S. Fahey. ‘Plant-soilmicrobial interactions in a northern hardwood forest’.. D. 49. 54.. ‘Annual nitrous oxide fluxes from temperate forest soils in the northeastern United States’. T. Bohlen. P. Pattern and Process in a Forested Ecosystem... A.: 1997. Beaty. Rep. R.. and Michel.: 1990. J. R. ‘Inorganic N losses from a forested ecosystem in response to physical. 9. M.: 1995. H. 23–59. R. 965–978. Appl. M..A. Res. 43. P. ‘Effects of multiple fires on nutrient yields from streams draining boreal forest and fen watersheds: Nitrogen and phosphorus’. ‘Nutrient losses after clear-cut logging and slash burning in the Oregon Coast Range’. Snyder. L. Burns. Clarke.. J. 584–596. 30.. Bowden.: 1997. P. ‘Nitrogen retention capacity of a northern hardwood forest soil under ammonium sulfate additions’. Edgerton. Ecol. 185–197. Likens. and Bosatta. 34. 249–279. C. and Ingersoll. J. and locust: Evidence from the sandbox ecosystem study’. J. Atmos. M. 31. B. Buso. D. I. T. ‘Dissolved organic nitrogen budgets for upland. S. J. D. P. Soil Biol.: 1984. A. P.. Ecol.: 2002. T. Water Resour. F. M. and Martin. M. P.’. Vermont. ‘Potential for Acidification of Six Remote Ponds in the White Mountains of New Hampshire’. R. P. S. and Likens. Y. Murdoch. ‘Patterns of streamwater acidity in the Lye Brook Wilderness Area.: 1973. 119.: 1993. R.: 2000. Ollinger. C. Fish. Geophys. and Kochenderfer. Pierce. L. B.: 1998. W.: 1997. T. Angradi.: 1998. R. S. Rev. B. C. H. Hornbeck. Parker. Bormann. U. biotic and climatic perturbations’. V. D. N. 253.S. J. Sci.NITROGEN INPUT-OUTPUT BUDGETS 393 Aber. Environ. Ecosystems 5. W. and McDowell. pp. S. Environ. J. Bayley. and Likens. B. SpringerVerlag. Res. G. Campbell. Bowden. Sci. Ågren.: 1988.. 95. Holmes. J. R. C. D. ‘Input-output budgets of major ions for a forested watershed in western Maryland’. Manage. H. Ann. Groffman.. Zhang. chemical.. E. Shanley. Water. Lawrence. Earth Planet. 1450–1453. Bowden. W. G. E.: 1979. K. 3105–3120. S. E. Ecology 74. ‘Gaseous nitrogen emissions from undisturbed terrestrial ecosystems: An assessment of their impacts on local and global nitrogen budgets’. forested ecosystems in New England’. C. and Goodale... Adams. F. Bowden. J. D. Pollut. Biogeochemistry 49. Freuder.: 1986. Ashby. 25. No. 802–812.’. Hamburg. G. Gahler. 648–658. F. C. 95. G. . G.. W. 5... ‘Stream water and soil solution responses to 5 years of nitrogen and sulfur additions at the Fernow Experimental Forest.. Schindler. Aquat. 121–137. T.

M. M. 1051– 1062. Res. Lawrence.. A. D. H. Galloway. M. M. K. C.2.: 1999. B. Buso. E. J. R. A. 196–205. J..: 1998. M. Durham. ‘BROOK90: A Simulation Model for Evaporation. Forest Service. J.394 J. B.: 1999. L. N. N.. Ecol.S. M. Schofield. ‘Simulated streamflow response to possible differences in transpiration among species of hardwood trees’. 30.. Gilliam. Seely-Reynolds. Manage. Res. Smith. L. Pollut....: 2001. W. R.: 1997. Hornbeck. 26. W. Holloway. Peters. 20. R. Pollut. New Hampshire’. D. J.: 1995. Adams. Environ. F. F. I. ‘Nitrogen leaching from European forests in relation to nitrogen deposition’. BioScience 51. A. West Virginia’. P. W. C. Monit. Res. 435–436. Kahl. Mitchell. B.. J. ‘Application of kriging to estimating mean annual precipitation in a region of orographic influence’. SAF Publ. F. D. Soil Water. Abundant Opportunities. 433–450.. 36.: 1997. Cronan. and Lash. 113–131. 1595–1602. B. CAMPBELL ET AL. Environ. ‘Eastern Forest Fires can have Long-term Impacts on Nitrogen Cycling’.. 153–161. ‘Acidic deposition in the northeastern United States: Sources and inputs. 31. L. 55–64. and Dahlgren. 73–89. 71. Ecol. L. B. J. ‘Long-term ionic increases from a central Appalachian forested watershed’. and Helvey. S.. and Johannes.. J. B. S. J. Eagar. Federer. C. Qual. For. C.: 2001. R.. Nature 395.: 1991. G. M.: 1990. N. 15–24. Albuquerque. S. ‘Ecosystem nutrient responses to chronic nitrogen inputs at Fernow Experimental Forest. Hornbeck. B. Callesen. Ito. Lambert. S. W. 102. 97-03. Fernandez. J.. Galloway.: 1978. H. J. Geology 27. Likens. For. B. Martin. S. H.: 1998. C. M. Res.. 1089–1097. Rustad. D. P. New York’. I. ‘The long-term effects of disturbance on organic and inorganic nitrogen export in the White Mountains. W. W. Can. Environ. J. C. J. 250–255. G. 329–339. T. B. A. and Shanley. and deVries. 567–570. J. 93. Hornbeck. and Reynolds. and Streamflow. Bull. 55.: 1996.: 2000. in Diverse Forests. Environ. and McDowell. Dise.. M. 403–407. Holloway. Yurish.. G. Driscoll. C. L. and Casey. W. ‘Processes and causes of lake acidification during spring snowmelt in west-central Adirondack Mountains. ‘Effects of intensive harvesting on nutrient capitals of three forest types in New England’. E. C. Water Resour. 24. Version 3. and management strategies’. and Handley. ecosystem effects. L. Environ. Edwards. G. Gundersen.: 1988. Department of Agriculture. 102. J. NH 03824. Computer Freeware and Documentation’. Can. Ecosystems 3. 180–198. T. J.. C. Hendrey. ‘Contribution of bedrock nitrogen to high nitrate concentrations in stream water’. R. C. 1768–1785. Proceedings 1996 Society of American Foresters Convention. and Evolving Realities. Gilliam.. Dingman. J. pp.: 1998. K. Ecol. Assess. M. . C. NM. F. ‘Temporal and spatial variation of nitrogen transformations in nitrogen-saturated soils of a central Appalachian hardwood forest’. C. and Pierce. For. J. ‘Nitrate leaching in forest ecosystems is related to forest floor C/N ratios’. Bear Brook Watershed in Maine (BBWM)’.. Bailey.. N. C.O. and Wright. ‘Streamwater chemistry and nutrient budgets for forested watersheds in New England: variability and management implications’. Can. Northeastern Forest Experiment Station. R. Federer. For. W. Stoddard. T. Tritton. T. Butler. Goodale. U.: 2002. Norton.. Dahlgren. 785–788. M. Box 640. 9–13 November.. Manage.. J. A. and Adams. Aber. P. S. ‘Geologic nitrogen in terrestrial biogeochemical cycling’. and Lawrence. L. Hansen. ‘Nitrogen and sulfur inputoutput budgets in the experimental and reference watersheds. Water Resour. Bulger. For. D. ‘Spatial patterns of precipitation quantity and chemistry and air temperature in the Adirondack region of New York’. and Weathers. S. Manage. A...: 1987.. and Yurish. 44. 14. For. Atmos. J. ‘The global nitrogen cycle: Changes and consequences’.: 1997. J. and Dricsoll.

H. M.. Mitchell. Nadelhoffer.. Appl. G.. McDowell. and Lindberg. S. pp. U. 84. 109–121.. S. J. Nadelhoffer. G. Res.. M. Environ. Res. P. D. S. T.A..: 1983. Arons. Driscoll. For. Sci. Technol. E. K.. and Eisenreich. 3305–3307... C. McNulty. H. Melillo. Lovett. C. E. 565–568. . A. M. and Bormann. ‘Nitrogen biogeochemistry of three hardwood ecosystems in the Adirondack Mountains of New York’. J. U. J..’..: 2000. 36. D. ‘Hydrologic control of sulfate mobility in a forested watershed’. 159. and Sobczak. Process.. 32A–42A. and Raynal. Hydrol. M. C. Schaefer. D. NY. P. ‘Spatial changes in forest floor and foliar chemistry of spruce-fir forests across New England’. J. ‘Long-term nitrogen additions and nitrogen saturation in two temperate forests’. J. Biogeochemistry of a Forested Ecosystem. J. 1642–1647. J. P. M. 3091–3094. C. S. L. Inamdar. D. G.: 1993. E. Weathers. Ecosystems 3..: 1995.: 2000. ‘Soil nitrogen transformations in beech and maple stands along a nitrogen deposition gradient’. J. Technol. ‘Changes in streamwater chemistry after 20 years from forested watersheds in New Hampshire. M. and Steudler. Atmos..: 1990. 32. A. K. W.’. F. J.: 1993. Res.: 2000. Battles. Can. Likens.: 1996. Atmos. H. and Aber. Lovett. J. 1695–1703. Kahl. Likens. Water Resour.. Magill.. V. J.: 2001a. Biogeochemistry 28. Technol. B. J. M. and Corbett. 27. Biogeochemistry 14. B. T. Sci.: 2000. 9. J. Biogeochemistry 48. Sci. and Raynal. J. 24. Owen. Seely.S. W. J.A. Mitchell. 13–29. P. 93–133. H.: 1995. and Stoddard. Hydrol. 17. New York’. 73–84. S.. ‘Relation of climate change to the acidification of surface waters by nitrogen deposition’. J. Aber. S.: 1996. Manage. Ecol. S. Biogeochemistry 56. J.. J. Environ. T. 165–184. J. J. S. McNulty. M. K. J. Sci. A. E. 15. Fernandez. C. T. K. H. Mitchell. ‘The role of nitrate in the acidification of streams in the Catskill Mountains of New York’. D.: 1991. D. Driscoll. Lewis.: 1993. 1951–1965. 238–253. E. and Likens. ‘Atmospheric deposition and canopy interactions of nitrogen in forests’.. Environ. K. W. and Kinsman. A. J. Michener. and Valiela. M.: 1989. G. A.. C. Technol. 33–54. Mitchell. McHale. J. R. 25. I. ‘Retention and leaching losses of atmospherically-derived nitrogen in the aggrading coastal watershed of Waquoit Bay. 30. J. Res.S.A. G. 1330–1344. ‘Nitrogen solutes in an Adirondack forested watershed: Importance of dissolved organic nitrogen’. Ecol.: 2001. McDonnell. 1603–1616.. R. For. J. and Fahey. 2767–2786.’. ‘Experimental inducement of nitrogen saturation at the watershed scale’. Friedland.. D. Miller. Environ.: 1992. D. ‘Low stream nitrate concentrations associated with oak forests on the Allegheny High Plateau of Pennsylvania’. ‘Atmospheric pollutant deposition to high-elevation ecosystems’. T.. ‘Nitrogen saturation and retention in forested watersheds of the Catskill Mountains. 15. ‘Climatic control of nitrate loss from forested watersheds in the northeast United States’. Water Resour. J. Aber. Environ. and Boone. Murdoch. G. Lovett.. E. ‘Role of within lake processes and hydrobiogeochemical changes over 16 yr in a watershed in the Adirondack Mountains of New York State. J. Lovett. New York. and Lawrence. A. and Johnson. S. V. H. and Rueth. J. Mitchell.: 2000.. ‘Linkages of nitrate losses in watersheds to hydrological processes’. Aber. P.. Driscoll. L. G. A. Murdoch.. ‘Nitrogen saturation in a high elevation New England spruce-fir stand’. G. D. Munger.. M. Process. 30. Burns. G. ‘Atmospheric deposition to forests along an elevational gradient at Whiteface Mountain. J. Mohnen. For. E. Martin. ‘Continental-scale variations in precipitation chemistry’. S. 23.S. D. and Pardo. A. Environ. M. Norton. Driscoll... D. J. 2121–2136. 27A.: 1998. Lynch. Berntson. U.: 1999. MA’. S.: 2001b. J. 28. S. J. J.. M. Panek. 10. Springer-Verlag. P. Res. Ecol.. Murdoch. A. Can. G. S. 2707–2720. and Newman. 2609–2612. G. P. and Cirmo. Appl. W. Water Resour. G. Lajtha. S. 1–8. C. Kadlecek..NITROGEN INPUT-OUTPUT BUDGETS 395 Kahl. McHale. I. J.

W. R. A.: 1996. Baker (ed. F. Appl. D. and Peters. G. Fry. Appl. T. Res. A. S. pp 250. F. Murdoch. E. 389–407. P.. Fish. A.. J. S. Tech.S.: 1988. Pollut. in L. Environ. ‘Effects of a windstorm and forest fire on chemical losses from forested watersheds and on the quality of receiving streams’. B. pp. Thesis. Christ. Keene. Hydrol. 1018–1026. P. BioScience 25. Can. E. T. Foster. Peterjohn. and Adams.: 2002. Weathers. 11. C. R. Wigington. and Reiners. A. C. ‘The fate of 15 N-labelled nitrate additions to a northern hardwood forest in eastern Maine. and Baker. R. 7. W. H. PA: U. D.. J.. and Lathrop. Aber. Swistock. C. McDowell. R. 22. Nelson. Skeffington. 112. 580– 588. M. J. M.. 376–381. J.396 J. For. Radnor. 119. S. NADP: 2002. J.. and Tarrant. 655–669. R. V.. G. W. CAMPBELL ET AL.. H. Adams. Eaton. J.: 1978. ‘Episodic acidification of small streams in the northeastern United States: Ionic controls of episodes’. and Adams. J. Bormann. and Wilson.. McGervey. Biogeochemistry 3. Forest Service. T. Stoddard. G. M. K. J. W. Edwards. D. Process. 37. Can. G. pp. J. Aber.’. J. ‘Modeling physical and chemical climate of the northeastern United States for a geographic information system’. A.: 1996.: 1999. 528–540. J. Smiley. 292–301. J. T. Sci. K. R. F. Driscoll. M. D. ‘Long-term Changes in Watershed Retention of Nitrogen’. IL 61820. Bicknell. ‘Symptoms of nitrogen saturation in two central Appalachian hardwood forest ecosystems’. ‘Stream chemistry and watershed nutrient economy following wildfire and fertilization in eastern Washington’.. M. Kluwer Academic Publishers. N. 649–663. Federer.. Downs. and DeWalle. K.. Peterjohn. A.. C.: 1997. C. Technol.S. A. Biogeochemistry 35.. American Chemical Society. Galloway. B. 507–522. L. The Bear Brook Watershed in Maine: A Paired Watershed Experiment – The First Decade (1987–1997). Aquat. C.. C. Norton. Prokopowich. W. S. 6. Nadelhoffer. 28.. National Atmospheric Deposition Program (NRSP-3)/National Trends Network. .: 1999. Helvey. Wood. Illinois State Water Survey. R. S. ‘Nitrous oxide production in two forested watersheds exhibiting symptoms of nitrogen saturation’. B.. Lovett. Gen. 2204 Griffith Drive. U. Northeastern Forest Experiment Station. Van Sickle.. A. R. Ecol. J. T. Oecologia 103. L. Peterjohn. M. J.. G.: 1988. ‘Comparison of methods for calculating annual solute exports from six forested Appalachian watersheds’. M. Kimball. Sexstone. 328–334. P. 209–224. and Anderson. H. D.S. D. ‘The effect of landscape features on deposition to Hunter Mountain. ‘Ecosystem succession and nutrient retention: A hypothesis’. Tiedemann.. D. M.: 1976.. J. T.). Ollinger. 223–284. University of Maine. Magill.. A. Foster. Weathers.A. Lovett. Likens.. J. E. A. B. M. J. J.. Wright. 54. C. D. N. I. Daube. Ecol. P. and Melillo. J. W. B. and Gilliam. 1723–1732. R.: 1995.. E. R. p. J.. S.. Qual. J.. C. A. Simonin. and Dalton. J. J. ‘Concentration and flux of solutes from snow and forest floor during snowmelt in the West-Central Adirondak region of New York’. Champaign. B. A. K. K. G..C. 30. Catskill Mountains.. T..: 1980.: 1975. M. M. and Fernandez.. T. D. Siccama. S.. Rep.. Ecology 57.. M. Boston.. Vitousek.: 1994. J. Ruszczynski. W. Bormann. H. Sci. Ecol. J.. ‘Patterns of nitrogen availability within a forested watershed exhibiting symptoms of nitrogen saturation’. J. Environmental Chemistry of Lakes and Reservoirs. ‘Excess nitrogen deposition: Issues for consideration’. P. 159–184.. M. NADP Program Office. 10. For. Rascher.. Department of Agriculture. Environ..: 1995. B.: 1987. ‘The impact of forest fire on the nutrient influxes to small lakes in northeastern Minnesota’. Environ. Manage. ‘Determining Atmospheric Inputs to Two Small Watersheds at Acadia National Park’. 247–257. DeWalle. W.: 1998. Christ. J. Kretser. D. Beaty. and Ellis.. H. Newbury. New York’.. W. F. Schindler. R. NE-191. ‘Cloudwater chemistry from ten sites in North America’. Washington.: 2000. Likens.