BACKGROUND AEROSOL IN THE UNITED STATES: NATURAL SOURCES AND TRANSBOUNDARY POLLUTION Daniel J. Jacob and Rokjin J. Park with support from EPRI, EPA/OAQPS.

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BACKGROUND AEROSOL IN THE UNITED STATES: NATURAL SOURCES AND TRANSBOUNDARY POLLUTION Daniel J. Jacob and Rokjin J. Park with support from EPRI, EPA/OAQPS How good are the “default estimated natural PM concentrations” proposed by EPA as 2064 endpoint for application of the Regional Haze Rule? To what extent does transboundary pollution compromise achievability of natural PM concentrations?

EMISSION REDUCTIONS FOR THE RHR ARE STRONGLY SENSITIVE TO CHOICE OF 2064 ENDPOINT Conceptual calculation for mean western U.S. conditions, assuming linear relationship between emissions and b ext Desired trend in visibility Required % decrease of U.S. anthropogenic emissions Phase 1 30% 48%

STRATEGY FOR QUANTIFYING BACKGROUND PM CONCENTRATIONS IN UNITED STATES Quantify natural aerosol concentrations Quantify transboundary pollution Start from best a priori estimates of natural and anthropogenic PM sources Simulate PM concentrations with GEOS-CHEM global model Evaluate with observations from IMPROVE, CASTNET, other networks Improved emission estimates Conduct sensitivity simulations

GEOS-CHEM GLOBAL CHEMICAL TRANSPORT MODEL ( Driven by NASA/GEOS-3 assimilated meteorological data with 2 o x2.5 o horizontal resolution, 48 levels in vertical Carbonaceous aerosol simulation (OC, EC) for 1998 Park, R.J., D.J. Jacob, M. Chin, and R.V. Martin, Sources of carbonaceous aerosols over the United States: implications for natural visibility, J. Geophys. Res.., 108, 4355, Coupled oxidant –sulfate-nitrate-ammonium simulation for 2001 (also 1998) Park, R.J., D.J. Jacob, et al., Natural and transboundary influences on ammonium-sulfate-nitrate aerosols in the United States: implications for visibility, J. Geophys. Res., manuscript in preparation

CARBONACEOUS AEROSOL SIMULATION Best a priori sources (1998) ORGANIC CARBON (OC) ELEMENTAL CARBON (EC) GLOBAL UNITED STATES 130 Tg yr Tg yr Tg yr Tg yr -1

BIOMASS BURNING EMISSIONS IN GEOS-CHEM: Climatology from Duncan, Logan, et al. [JGR 2002] scaled to 1998 using TOMS and ATSR satellite data Interannual variability derived from TOMS Aerosol Index [Duncan et al., 2002] 1998 fires from ATSR satellite data: Apr-May fires in Mexico Jul-Sep fires in U.S/Canada

SEASONAL VARIATION OF OC AND EC Constrain OC/EC sources using simulation of monthly mean IMPROVE observations and model tracers of individual source types. IMPROVE model model tracers (additive) biomass burning vegetation fossil fuel biofuel

LEAST-SQUARES FIT OF MODEL TO MONTHLY MEAN OC/EC OBSERVATIONS AT 45 IMPROVE SITES YIELDS OPTIMIZED A POSTERIORI SOURCES Fossil fuel  15% Biofuel  65% Biomass burning  17% Biogenic  11%

CARBONACEOUS AEROSOL IN THE U.S.: contributions from natural sources and transboundary pollution OC (  g m -3 as OMC) West East EC (  g m -3 ) West East Baseline (1998) Background (no U.S. anthrop. emissions, climatological fires) Natural (no anthrop. emissions globally) Transboundary pollution enhancements Canada and Mexico Asia EPA default estimated natural concentrations Annual regional means from GEOS-CHEM standard and sensitivity simulations EPA default natural concentrations for OC are OK in eastern U.S., a factor of 2- 3 too low in western U.S. – quantifying fire influences is critical Transboundary pollution influences are relatively small

H 2 SO 4 -HNO 3 -NH 3 -H 2 O AEROSOL SIMULATION GEOS-CHEM emissions (2001) GLOBALUNITED STATES Sulfur, Tg S yr -1 Ammonia, Tg N yr -1 NO x, Tg N yr

ANNUAL MEAN SULFATE (2001): GEOS-CHEM vs. IMPROVE (141 sites) Highest concentrations in industrial Midwest (coal-fired power plants)

SULFATE AT IMPROVE, CASTNET, NADP (deposition) SITES: model vs. observed for different seasons High correlation, no significant model bias except 25-30% negative bias in summer (we attribute it to excessive scavenging of SO 2 in convective updrafts)

ANNUAL MEAN AMMONIUM (2001): GEOS-CHEM vs. CASTNET (79 sites) Highest concentrations in upper Midwest (livestock) (no ammonium data at IMPROVE sites)

ANNUAL MEAN NITRATE (2001): GEOS-CHEM vs. CASTNET (79 sites) Highest concentrations in upper Midwest (NH 4 NO 3 formation limited by ammonia availability)

AMMONIUM AND NITRATE AT CASTNET AND IMPROVE SITES: model vs. observed for different seasons Ammonium Nitrate Nitrate High bias for NH 4 + in fall: excessive seasonal livestock emissions High bias for NO 3 -, esp. in summer/fall, results from bias on [SO 4 2- ]-2[NH 4 + ]

SULFATE-NITRATE-AMMONIUM AEROSOL IN THE U.S.: contributions from natural sources and transboundary pollution Large transboundary pollution influence prevents achievability of natural concentrations; Transboundary pollution influence from Asia is comparable in magnitude to that from Canada + Mexico Annual regional means from GEOS-CHEM standard and sensitivity simulations Ammonium sulfate (  g m -3 ) West East Ammonium nitrate (  g m -3 ) West East Baseline (2001) Background (no U.S. anthrop. emissions) Natural (no anthrop. emissions globally) Transboundary pollution enhancements Canada and Mexico Asia EPA default estimated natural concentrations

MODEL EVALUATION WITH ASIAN OUFLOW OBSERVATIONS OF SULFATE FROM TRACE-P AIRCRAFT CAMPAIGN (MAR-APR 2001) model obs Observations from Jordan et al. [[JGR 2003]

INTERCONTINENTAL TRANSPORT OF ASIAN AND NORTH AMERICAN ANTHROPOGENIC SULFATE As determined from GEOS-CHEM 2001 sensitivity simulations with these sources shut off Asian anthropogenic sulfate N. American anthropogenic sulfate