Natural and transboundary pollution influences on sulfate‐nitrate‐ammonium aerosols in the United States: Implications for policy

[1] We use a global three-dimensional coupled oxidant-aerosol model (GEOS-CHEM) to estimate natural and transboundary pollution influences on sulfate-nitrate-ammonium aerosol concentrations in the United States. This work is motivated in part by the Regional Haze Rule of the U.S. Environmental Protection Agency (EPA), which requires immediate action to improve visibility in U.S. wilderness areas along a linear trajectory toward an endpoint of “natural visibility conditions” by 2064. We present full-year simulations for 1998 and 2001 and evaluate them with nationwide networks of observations in the United States and Europe (Interagency Monitoring of Protected Visual Environments (IMPROVE), Clean Air Status and Trends Network (CASTNET), National Atmospheric Deposition Program (NADP), European Monitoring and Evaluation Programme (EMEP)) and with Asian outflow observations from the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission. Shutting off U.S. anthropogenic emissions in the model defines “background” aerosol concentrations representing contributions from both natural and transboundary pollution sources. We find that transboundary transport of pollution from Canada, Mexico, and Asia dominates over natural influences for both sulfate and nitrate. Trans-Pacific transport of Asian pollution accounts for 30% of background sulfate in both the western and eastern United States. Our best estimates of natural concentrations for ammonium sulfate and ammonium nitrate in the United States are either consistent with or lower than the default values recommended by EPA for natural visibility calculations. However, the large transboundary pollution influence in our calculation suggests that a natural visibility objective cannot be approached without international emission controls.

[1]  Lorraine A. Remer,et al.  Cloud optical thickness feedbacks in the CO2 climate problem , 1984 .

[2]  R. Hirsch,et al.  METHODS OF FITTING A STRAIGHT LINE TO DATA: EXAMPLES IN WATER RESOURCES , 1984 .

[3]  M. Molina,et al.  Chemical kinetics and photochemical data for use in stratospheric modeling , 1985 .

[4]  L. Merlivat,et al.  Air-Sea Gas Exchange Rates: Introduction and Synthesis , 1986 .

[5]  D. Jacob Chemistry of OH in remote clouds and its role in the production of formic acid and peroxymonosulfate , 1986 .

[6]  P. Buat-Ménard The role of air-sea exchange in geochemical cycling , 1986 .

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

[8]  J. Kristjánsson,et al.  Condensation and Cloud Parameterization Studies with a Mesoscale Numerical Weather Prediction Model , 1989 .

[9]  P. Crutzen,et al.  Are there interactions of iodine and sulfur species in marine air photochemistry , 1990 .

[10]  W. Freas,et al.  National air quality and emissions trends report, 1989. Executive Summary and Chapter 4 - excerpts , 1991 .

[11]  W. Malm,et al.  Spatial and seasonal trends in particle concentration and optical extinction in the United States , 1994 .

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

[13]  Mian Chin,et al.  Anthropogenic and natural contributions to tropospheric sulfate: A global model analysis , 1996 .

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

[15]  Mian Chin,et al.  A global three‐dimensional model of tropospheric sulfate , 1996 .

[16]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1997 .

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

[18]  Spyros N. Pandis,et al.  Response of Inorganic PM to Precursor Concentrations , 1998 .

[19]  R. Andres,et al.  A time‐averaged inventory of subaerial volcanic sulfur emissions , 1998 .

[20]  Global simulation of tropospheric O3-NOx-hydrocarbon chemistry: 1. Model formulation , 1998 .

[21]  J. Logan,et al.  Effect of rising Asian emissions on surface ozone in the United States , 1999 .

[22]  S. Pandis,et al.  Marginal PM25: Nonlinear Aerosol Mass Response to Sulfate Reductions in the Eastern United States. , 1999, Journal of the Air & Waste Management Association.

[23]  Giacomo R. DiTullio,et al.  A global database of sea surface dimethylsulfide (DMS) measurements and a procedure to predict sea surface DMS as a function of latitude, longitude, and month , 1999 .

[24]  Daniel A. Jaffe,et al.  Influence of Asian emissions on the composition of air reaching the north western United States , 1999 .

[25]  John H. Seinfeld,et al.  Global concentrations of tropospheric sulfate, nitrate, and ammonium aerosol simulated in a general circulation model , 1999 .

[26]  Itsushi Uno,et al.  Transport of Asian air pollution to North America , 1999 .

[27]  Mian Chin,et al.  Atmospheric sulfur cycle simulated in the global model GOCART: Comparison with field observations and regional budgets , 2000 .

[28]  D. Jacob Heterogeneous chemistry and tropospheric ozone , 2000 .

[29]  D. Jacob,et al.  Transport and scavenging of soluble gases in a deep , 2000 .

[30]  Viney P. Aneja,et al.  Characterization of atmospheric ammonia emissions from swine waste storage and treatment lagoons , 2000 .

[31]  Joshua P. Hacker,et al.  Long‐range transport of Asian dust to the Lower Fraser Valley, British Columbia, Canada , 2001 .

[32]  D. Jacob,et al.  Constraints from 210Pb and 7Be on wet deposition and transport in a global three‐dimensional chemical tracer model driven by assimilated meteorological fields , 2001 .

[33]  D. Jacob,et al.  Asian chemical outflow to the Pacific in spring: Origins, pathways, and budgets , 2001 .

[34]  D. Jacob,et al.  Global modeling of tropospheric chemistry with assimilated meteorology : Model description and evaluation , 2001 .

[35]  Bryan N. Duncan,et al.  A tropospheric ozone maximum over the Middle East , 2001 .

[36]  D. Finn,et al.  April 1998 Asian dust event over the Columbia Plateau , 2001 .

[37]  J. Seinfeld,et al.  General circulation model assessment of direct radiative forcing by the sulfate-nitrate-ammonium-water inorganic aerosol system , 2001 .

[38]  C. Land,et al.  A comparison of large-scale atmospheric sulphate aerosol models (COSAM): overview and highlights , 2001 .

[39]  Robert Frouin,et al.  Asian Dust Events of April 1998 , 2001 .

[40]  M. Andreae,et al.  Emission of trace gases and aerosols from biomass burning , 2001 .

[41]  R. Martin,et al.  Sources of tropospheric ozone along the Asian Pacific Rim: An analysis of ozonesonde observations , 2002 .

[42]  R. Martin,et al.  Stratospheric versus pollution influences on ozone at Bermuda: Reconciling past analyses , 2002 .

[43]  D. Jacob,et al.  Background ozone over the United States in summer: Origin, trend, and contribution to pollution episodes , 2002 .

[44]  Paul Ginoux,et al.  Interpretation of TOMS observations of tropical tropospheric ozone with a global model and in-situ observations , 2002 .

[45]  L. Barrie,et al.  Canadian Aerosol Module (CAM): A size-segregated simulation of atmospheric aerosol processes for climate and air quality models 2. Global sea-salt aerosol and its budgets , 2002 .

[46]  Bryan N. Duncan,et al.  Transatlantic transport of pollution and its effects on surface ozone in Europe and North America , 2002 .

[47]  Robin L. Dennis,et al.  Seasonal NH3 emission estimates for the eastern United States , 2003 .

[48]  Paul A. Roelle,et al.  Characterization of ammonia emissions from soils in the upper coastal plain, North Carolina , 2002 .

[49]  F. Binkowski,et al.  Models-3 community multiscale air quality (cmaq) model aerosol component , 2003 .

[50]  D. Jacob,et al.  An intercomparison and evaluation of aircraft-derived and simulated CO from seven chemical transport models during the TRACE-P experiment , 2003 .

[51]  Merritt N. Deeter,et al.  Asian Outflow and Trans-Pacific Transport of Carbon Monoxide and Ozone Pollution: An Integrated Satellite, Aircraft, and Model Perspective , 2003 .

[52]  J. Seinfeld,et al.  Modification of aerosol mass and size distribution due to aqueous‐phase SO2 oxidation in clouds: Comparisons of several models , 2003 .

[53]  Bryan N. Duncan,et al.  Transport pathways for Asian pollution outflow over the Pacific: Interannual and seasonal variations , 2003 .

[54]  Jennifer A. Logan,et al.  An assessment of biofuel use and burning of agricultural waste in the developing world , 2003 .

[55]  D. Blake,et al.  Export of anthropogenic reactive nitrogen and sulfur compounds from the East Asia region in spring , 2003 .

[56]  R. Martin,et al.  Global and regional decreases in tropospheric oxidants from photochemical effects of aerosols , 2003 .

[57]  I. McKendry,et al.  Six 'new' episodes of trans-Pacific transport of air pollutants , 2003 .

[58]  R. Martin,et al.  Application of empirical orthogonal functions to evaluate ozone simulations with regional and global models , 2003 .

[59]  L. Jaeglé,et al.  PHOBEA/ITCT 2002 Airborne Observations of trans-Pacific Transport of Ozone, CO, VOCs, and Aerosols to the Northeast Pacific: Impacts of Asian Anthropogenic and Siberian Boreal Fire Emissions. , 2003 .

[60]  R. Martin,et al.  Interannual and seasonal variability of biomass burning emissions constrained by satellite observations , 2003 .

[61]  Michael Q. Wang,et al.  An inventory of gaseous and primary aerosol emissions in Asia in the year 2000 , 2003 .

[62]  Henry E. Fuelberg,et al.  Uptake of nitrate and sulfate on dust aerosols during TRACE‐P , 2003 .

[63]  John C. Gille,et al.  Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission: Design, execution, and first results , 2003 .

[64]  Mian Chin,et al.  Sources of carbonaceous aerosols over the United States and implications for natural visibility , 2003 .

[65]  Mian Chin,et al.  Effects of the physical state of tropospheric ammonium-sulfate-nitrate particles on global aerosol direct radiative forcing , 2003 .

[66]  G. Carmichael,et al.  Dynamics and transport of sulfur dioxide over the Yellow Sea during TRACE-P , 2003 .

[67]  Arlene M. Fiore,et al.  Variability in surface ozone background over the United States: Implications for air quality policy , 2003 .

[68]  Dylan B. A. Jones,et al.  Inverting for emissions of carbon monoxide from Asia using aircraft observations over the western Pacific , 2003 .

[69]  D. Jacob,et al.  Sources and budgets for CO and O3 in the northeastern Pacific during the spring of 2001: Results from the PHOBEA‐II Experiment , 2003 .

[70]  D. Jacob,et al.  A global three-dimensional model analysis of the atmospheric budgets of HCN and CH 3 CN: Constraints from aircraft and ground measurements , 2003 .

[71]  Heather Price,et al.  PHOBEA/ITCT 2002 airborne observations of transpacific transport of ozone, CO, volatile organic compounds, and aerosols to the northeast Pacific: Impacts of Asian anthropogenic and Siberian boreal fire emissions , 2004 .

[72]  D. Jacob,et al.  Export of NOy from the North American boundary layer: Reconciling aircraft observations and global model budgets , 2004 .

[73]  D. Jacob,et al.  Constraints on the sources of tropospheric ozone from 210Pb-7Be-O3 correlations , 2004 .

[74]  David G. Streets,et al.  Improved quantification of Chinese carbon fluxes using CO2/CO correlations in Asian outflow , 2004 .

[75]  David G. Streets,et al.  Constraints on Asian and European sources of methane from CH4‐C2H6‐CO correlations in Asian outflow , 2004 .

[76]  Peter H. McMurry,et al.  Particulate Matter Science for Policy Makers , 2005 .