NITROGEN DEPOSITION ONTO THE UNITED STATES AND WESTERN EUROPE: SYNTHESIS OF OBSERVATIONS AND MODELS

The documented acceleration of NH3 and NOx (NO NO2) emissions over the last 150 years has accelerated N deposition, compromising air and water quality and altering the functioning of terrestrial and aquatic ecosystems worldwide. To construct con- tinental-scale N budgets, we produced maps of N deposition fluxes from site-network observations for the United States and Western Europe. Increases in the rates of N cycling for these two regions of the world are large, and they have undergone profound modification of biospheric-atmospheric N exchanges, and ecosystem function. The maps are necessarily restricted to the network measured quantities and consist of statistically interpolated fields of aqueous NO3 and NH4, gaseous HNO3 and NO2 (in Europe), and particulate NO3 and NH4. There remain a number of gaps in the budgets, including organic N and NH3 de- position. The interpolated spatially continuous fields allow estimation of regionally inte- grated budget terms. Dry-deposition fluxes were the most problematic because of low station density and uncertainties associated with exchange mechanisms. We estimated dry N de- position fluxes by multiplying interpolated surface-air concentrations for each chemical species by model-calculated, spatially explicit deposition velocities. Deposition of the ox- idized N species, by-products of fossil-fuel combustion, dominate the U.S. N deposition budget with 2.5 Tg of NOy-N out of a total of 3.7-4.5 Tg of N deposited annually onto the conterminous United States. Deposition of the reduced species, which are by-products of farming and animal husbandry, dominate the Western European N-deposition budget with a total of 4.3-6.3 Tg N deposited each year out of a total of 8.4-10.8 Tg N. Western Europe receives five times more N in precipitation than does the conterminous United States. Estimated N emissions exceed measured deposition in the United States by 5.3- 7.81 Tg N, suggesting significant N export or under-sampling of urban influence. In Europe, estimated emissions better balance measured deposition, with an imbalance of between 0.63 and 2.88 Tg N, suggesting that much of the N emitted in Europe is deposited there, with possible N import from the United States. The sampling network in Europe includes urban influences because of the greater population density of Western Europe. Our analysis of N deposition for both regions was limited by sampling density. The framework we present for quantification of patterns of N deposition provides a constraint on our under- standing of continental biospheric-atmospheric N cycles. These spatially explicit wet and dry N fluxes also provide a tool for verifying regional and global models of atmospheric chemistry and transport, and they represent critical inputs into terrestrial models of bio- geochemistry.

[1]  W. Slinn,et al.  Predictions for particle deposition to vegetative canopies , 1982 .

[2]  Gary M. Lovett,et al.  Atmospheric Deposition of Nutrients and Pollutants in North America: An Ecological Perspective , 1994 .

[3]  F. Chapin,et al.  Biotic Control over the Functioning of Ecosystems , 1997 .

[4]  James N. Galloway,et al.  Nitrogen and phosphorus budgets of the North Atlantic Ocean and its watershed , 1996 .

[5]  Charles T. Driscoll,et al.  CAN SITE‐SPECIFIC TRENDS BE EXTRAPOLATED TO A REGION? AN ACIDIFICATION EXAMPLE FOR THE NORTHEAST , 1998 .

[6]  D. Jacob,et al.  The NO2 Flux Conundrum , 2000, Science.

[7]  M. Wesely,et al.  Measurements and parameterization of particulate sulfur dry deposition over grass , 1985 .

[8]  Scott V. Ollinger,et al.  SIMULATING OZONE EFFECTS ON FOREST PRODUCTIVITY: INTERACTIONS AMONG LEAF‐, CANOPY‐, AND STAND‐LEVEL PROCESSES , 1997 .

[9]  Robert Sausen,et al.  Estimations of global no, emissions and their uncertainties , 1997 .

[10]  B. Emmett,et al.  Nitrogen deposition makes a minor contribution to carbon sequestration in temperate forests , 1999, Nature.

[11]  R. Talbot,et al.  Summertime measurements of aerosol nitrate and ammonium at a northeastern U.S. site , 2001 .

[12]  D. Dunkerley Europe , 1993 .

[13]  J. Aber,et al.  Effects of land use, climate variation, and N deposition on N cycling and C storage in northern hardwood forests , 1997 .

[14]  Particle deposition to forests—Summary of results and application , 1997 .

[15]  F. Berendse,et al.  Competition and Nitrogen Loss from Plants in Grassland Ecosystems , 1992 .

[16]  D. Tilman,et al.  Influence of Nitrogen Loading and Species Composition on the Carbon Balance of Grasslands , 1996, Science.

[17]  William H. McDowell,et al.  Nitrogen Saturation in Temperate Forest Ecosystems , 1998 .

[18]  D. Schimel,et al.  Gaseous ammonia fluxes and background concentrations in terrestrial ecosystems of the United States , 1992 .

[19]  L. Kleinman,et al.  Ozone production efficiency in an urban area , 2002 .

[20]  M. Wesely Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models , 1989 .

[21]  I. Ilyin,et al.  Co-operative Programme for Monitoring and Evaluation of the Long-Range Transmission of Air Pollutants in Europe EMEP , 2001 .

[22]  P. Mayewski,et al.  An ice-core record of atmospheric response to anthropogenic sulphate and nitrate , 1990, Nature.

[23]  John L. Stoddard,et al.  Long-term changes in watershed retention of nitrogen, its causes and aquatic consequences , 1994 .

[24]  D. Fowler,et al.  The Exchange of Ammonia Between the Atmosphere and Plant Communities , 1993 .

[25]  G. Likens,et al.  Technical Report: Human Alteration of the Global Nitrogen Cycle: Sources and Consequences , 1997 .

[26]  William H. McDowell,et al.  The origin, composition and rates of organic nitrogen deposition: A missing piece of the nitrogen cycle? , 2002 .

[27]  E. Atlas,et al.  Observations of Ozone Formation in Power Plant Plumes and Implications for Ozone Control Strategies , 2001, Science.

[28]  D. Schimel,et al.  Terrestrial ecosystems and the carbon cycle , 1995 .

[29]  P. Reich,et al.  The Influence of Functional Diversity and Composition on Ecosystem Processes , 1997 .

[30]  V. L. Orkin,et al.  Scientific Assessment of Ozone Depletion: 2010 , 2003 .

[31]  G. Likens,et al.  Atmospheric dust and acid rain , 1996 .

[32]  E. Sanhueza,et al.  A Global Overview of Atmospheric Acid Deposition Fluxes , 1997 .

[33]  P. Kasibhatla,et al.  Year 2020: Consequences of population growth and development on deposition of oxidized nitrogen , 1994 .

[34]  Barry Lefer,et al.  Nitric acid and ammonia at a rural northeastern U.S. site , 1999 .

[35]  Ramakrishna R. Nemani,et al.  The VEMAP integrated database for modelling United States ecosystem/vegetation sensitivity to climate change , 1995 .

[36]  Ernst-Detlef Schulze,et al.  Carbon and Nitrogen Cycling in European Forest Ecosystems , 2000, Ecological Studies.

[37]  J. F. Clarke,et al.  Comparison of dry deposition velocities for SO2, HNO3 and SO42− estimated with two inferential models , 1996 .

[38]  P. Hanson,et al.  Dry deposition of reactive nitrogen compounds: A review of leaf, canopy and non-foliar measurements , 1991 .

[39]  R. Barthelmie,et al.  Nitrogen dry deposition at an AmeriFlux site in a hardwood forest in the midwest , 1999 .

[40]  Gary M. Lovett,et al.  Atmospheric deposition and canopy interactions of nitrogen in forests , 1993 .

[41]  J. Lynch,et al.  Changes in sulfate deposition in eastern USA following implementation of Phase I of Title IV of the Clean Air Act Amendments of 1990. , 2000 .

[42]  C. Field,et al.  Interactions of the major biogeochemical cycles : global change and human impacts , 2003 .

[43]  J. Schnoor,et al.  Nitrogen fixation: Anthropogenic enhancement‐environmental response , 1995 .

[44]  D. Powlson,et al.  Nitrogen deposition and carbon sequestration , 1999, Nature.

[45]  R. Aerts,et al.  Competition in heathland along an experimental gradient of nutrient availability , 1990 .

[46]  P. Vitousek,et al.  The Effects of Plant Composition and Diversity on Ecosystem Processes , 1997 .

[47]  J. Sulzman,et al.  Contemporary and pre-industrial global reactive nitrogen budgets , 1999 .

[48]  Thomas E. Graedel,et al.  Global gridded inventories of anthropogenic emissions of sulfur and nitrogen , 1996 .

[49]  C. Johansson Pine forest: a negligible sink for atmospheric NOx in rural Sweden , 1987 .

[50]  J. Aber,et al.  PLANT AND SOIL RESPONSES TO CHRONIC NITROGEN ADDITIONS AT THE HARVARD FOREST , 1993 .

[51]  P. Crutzen,et al.  A three-dimensional model of the global ammonia cycle , 1994 .

[52]  J. Erisman,et al.  Atmospheric deposition in relation to acidification and eutrophication , 1995 .

[53]  B. Lefer The chemistry and dry deposition of atmospheric nitrogen at a rural site in the northeastern United States , 1997 .

[54]  N. Cape Atmospheric deposition in relation to acidification and eutrophication (Studies in environmental science 63): By J. W. Erisman and G. P. J. Draaijers. Elsevier Science BV, Amsterdam, 1995, ISBN 0-444-82247-X, 442 pp. Price: US$161.75 , 1996 .

[55]  Dennis P. Swaney,et al.  Regional nitrogen budgets and riverine N & P fluxes for the drainages to the North Atlantic Ocean: Natural and human influences , 1996 .

[56]  D. Schimel,et al.  Atmospheric Chemistry and Greenhouse Gases , 1999 .

[57]  Jennifer A. Logan,et al.  Trends in the vertical distribution of ozone: An analysis of ozonesonde data , 1994 .

[58]  L. Barrie,et al.  An estimate of the importance of dry deposition as a pathway of acidic substances from the atmosphere to the biosphere in eastern Canada , 1988 .

[59]  J. Erisman,et al.  Review of deposition monitoring methods , 1994 .

[60]  Gene E. Likens,et al.  Steep declines in atmospheric base cations in regions of Europe and North America , 1994, Nature.

[61]  J. Melillo,et al.  The potential storage of carbon caused by eutrophication of the biosphere , 1985 .

[62]  Jean-Francois Lamarque,et al.  Variations in the predicted spatial distribution of atmospheric nitrogen deposition and their impact on carbon uptake by terrestrial ecosystems , 1997 .

[63]  M. Hauhs,et al.  Critical loads for nitrogen deposition on forest ecosystems , 1989 .

[64]  D. Imre,et al.  NO y lifetimes and O3 production efficiencies in urban and power plant plumes: Analysis of field data , 2000 .

[65]  E. Matthews Nitrogenous fertilizers: Global distribution of consumption and associated emissions of nitrous oxide and ammonia , 1994 .

[66]  J. Aber,et al.  Forest biogeochemistry and primary production altered by nitrogen saturation , 1995 .

[67]  Vaclav Smil,et al.  Global Population and the Nitrogen Cycle , 1997 .

[68]  J. M. Ellis,et al.  A Spatial Model of Atmospheric Deposition for the Northeastern U.S. , 1993, Ecological applications : a publication of the Ecological Society of America.

[69]  R. Jonas,et al.  Studies on the dry deposition of aerosol particles on vegetation and plane surfaces , 1985 .

[70]  B. Hicks,et al.  A review of the current status of knowledge on dry deposition , 2000 .

[71]  H. Sievering Nitrogen deposition and carbon sequestration , 1999, Nature.

[72]  Joyce E. Penner,et al.  Spatial and Temporal Patterns in Terrestrial Carbon Storage Due to Deposition of Fossil Fuel Nitrogen , 1996 .

[73]  Vanessa M. Loaiza,et al.  DATA REPORT , 2004 .

[74]  T. Meyers,et al.  Estimation of dry deposition velocity using inferential models and site-specific meteorology: Uncertainty due to siting of meteorological towers , 1997 .

[75]  G. Kramm,et al.  Determination of HNO3 dry deposition by modified Bowen ratio and aerodynamic profile techniques , 1993 .

[76]  K. E. Moore,et al.  Atmospheric deposition of reactive nitrogen oxides and ozone in a temperate deciduous forest and a subarctic woodland , 1996 .

[77]  C. Johansson,et al.  Dry deposition of nitrogen dioxide and ozone to coniferous forests , 1993 .

[78]  J. Duyzer,et al.  Assessment of dry deposition fluxes of NH3 and NH4+ over natural terrains , 1987 .

[79]  D. Schindler,et al.  Effects of Acid Rain on Freshwater Ecosystems , 1988, Science.

[80]  D. Fahey,et al.  Ozone production in the rural troposphere and the implications for regional and global ozone distributions , 1987 .

[81]  J. Aber,et al.  Nitrogen saturation in northern forest ecosystems , 1989 .

[82]  J. Lamarque,et al.  of the different nitrogen sources in the troposphere , 1996 .

[83]  J. Lelieveld,et al.  Dry deposition parameterization in a chemistry general circulation model and its influence on the distribution of reactive trace gases. , 1995 .

[84]  P. Reich,et al.  Interactive effects of nitrogen deposition, tropospheric ozone, elevated CO2 and land use history on the carbon dynamics of northern hardwood forests , 2002 .

[85]  J. Erisman,et al.  Mapping wet deposition of acidifying components and base cations over Europe using measurements , 1996 .

[86]  G. Heil,et al.  Atmospheric deposition and canopy exchange processes in heathland ecosystems. , 1992, Environmental pollution.

[87]  W. Parton,et al.  Agricultural intensification and ecosystem properties. , 1997, Science.

[88]  B. Hicks,et al.  Dry deposition inferential measurement techniques—I. Design and tests of a prototype meteorological and chemical system for determining dry deposition , 1991 .

[89]  W. Ruijgrok,et al.  The dry deposition of particles to a forest canopy: A comparison of model and experimental results , 1997 .

[90]  W. Cramer,et al.  The IIASA database for mean monthly values of temperature , 1991 .

[91]  Monitoring,et al.  Scientific assessment of ozone depletion: 1991 , 1992 .

[92]  J. F. Clarke,et al.  A multilayer model for inferring dry deposition using standard meteorological measurements , 1998 .

[93]  James N. Galloway,et al.  Atmospheric deposition of nutrients to the North Atlantic Basin. , 1996 .

[94]  D. Lamb,et al.  The national atmospheric deposition program: an overview. , 2000 .

[95]  J. William Munger,et al.  Regional budgets for nitrogen oxides from continental sources: Variations of rates for oxidation and deposition with season and distance from source regions , 1998 .

[96]  B. Emmett,et al.  reply: Nitrogen deposition and carbon sequestration , 1999, Nature.

[97]  Gene E. Likens,et al.  Long-Term Effects of Acid Rain: Response and Recovery of a Forest Ecosystem , 1996, Science.

[98]  S. Ollinger,et al.  Modeling nitrogen saturation in forest ecosystems in response to land use and atmospheric deposition , 1997 .

[99]  D. Kley,et al.  On the origin of tropospheric ozone , 1980 .

[100]  T. C. Haas,et al.  Kriging and automated variogram modeling within a moving window , 1990 .

[101]  T. C. Haas,et al.  Local Prediction of a Spatio-Temporal Process with an Application to Wet Sulfate Deposition , 1995 .

[102]  C. Field,et al.  Atmospheric chemistry and the bioatmospheric carbon and nitrogen cycles. , 2003 .

[103]  A. Bouwman,et al.  A global high‐resolution emission inventory for ammonia , 1997 .

[104]  W. J. Mitsch,et al.  Environmental Chemistry of Lakes and Reservoirs, Advances in Chemistry Series 237 , 1996 .

[105]  T. Lavery,et al.  Preliminary data from the USEPA dry deposition network: 1989. , 1992, Environmental pollution.

[106]  K. Peters,et al.  The dry deposition of gaseous and participate nitrogen compounds to a spruce stand , 1995 .

[107]  G. P. Wyers,et al.  Micrometeorological measurement of the dry deposition flux of sulphate and nitrate aerosols to coniferous forest , 1997 .

[108]  Richard D. Boone,et al.  Plant and Soil Responses to Chronic Nitrogen Additions at the Harvard Forest, Massachusetts. , 1993, Ecological applications : a publication of the Ecological Society of America.

[109]  C. Driscoll,et al.  Nitrogen cycling in forested catchments: A Chapman Conference , 1997 .