1. ASSESSING INTERCONTINENTAL TRANSPORT OF OZONE AND AEROSOLS AT NORTHERN MID-LATITUDES WITH GMI Daniel J. Jacob, Rokjin J. Park, Shiliang Wu, Colette L. Heald Project led by Jennifer A, Logan (P.I.)

2. New LRTAP/EMEP Task Force on Hemispheric Transport of Air Pollutants (HTAP) CHARGE: –develop a fuller understanding of the hemispheric transport of air pollution; – estimate the hemispheric transport of specific air pollutants for the use in reviews of protocols to the LRTAP Convention; –prepare technical reviews thereon for submission to the Steering Body of EMEP Chairs: Terry Keating (EPA) and Andre Zuber (Eur. Commission) First meeting: Brussels, Jun 1-3, 2005 Second meeting: Washington, DC, Jan 30-31, 2006 OBJECTIVES OF SECOND MEETING: Define model metrics for intercontinental transport of pollution; Develop potocols for model intercomparisons Coordinate modeling efforts, data bases;

3. TWO MODES OF INTERCONTINENTAL INFLUENCE AsiaN. America Europe Boundary layer Free troposphere liftingsubsidence boundary layer advection Tropopause HEMISPHERIC POLLUTION BACKGROUND “Direct” intercontinental transport Mixing Direct intercontinental transport: fast (~1 week) transport from source to receptor continent; either by boundary layer advection or by lifting to lower free troposphere followed by subsidence Hemispheric pollution: pollution mixes in free troposphere, affecting free tropospheric background, in turn affecting surface concentrations by subsidence 2 km

4. MECHANISM FOR TRANSPACIFIC TRANSPORT OF ANTHROPOGENIC OZONE AND AEROSOLS entrainment, dilution ASIA PACIFIC NORTH AMERICA NO x, SO 2, VOC warm conveyor belts, convection aerosols, HNO 3 PAN (~10%) VOCs (long-lived) OC aerosol PAN O3O3 NO x O3O3 Sulfate (10%) OC aerosol Boundary layer Free troposphere 2 km subsidence ozone, sulfate, OC HEMISPHERIC POLLUTION

5. MODEL METRIC FOR INTERCONTINENTAL INFLUENCE (1)Standard simulation; compare w/ observations (2) Set N. American anthropogenic emissions to zero  estimate background (3) Set global anthropogenic emissions to zero  estimate natural background Difference between (1) and (2)  regional pollution Difference between (2) and (3)  intercontinental pollution Could also apply small perturbations (e.g., 10%) to emissions from individual continents; to be discussed at HTAP workshop

6. Surface ozone at Voyageurs National Park, Minnesota (May-June 2001): simulations with GEOS-Chem CASTNet observations Model Background Natural Stratospheric + * Intercontinental pollution Regional pollution }  } Background: 15-36 ppbv Natural : 9-23 ppbv Stratosphere: < 7 ppbv X Fiore et al. [2003]

7. Probability distribution of afternoon (1-5 p.m. mean) surface ozone at U.S. CASTNet sites in March-October 2001 Probability. ppbv -1 CASTNet observations GEOS-Chem at CASTNet Natural 18±5 ppbv GEOS-Chem background 26±7 ppbv GEOS-Chem background 29±9 ppbv MOZART-2 Intercontinental pollution enhances background by 8 ± 4 ppbv relative to natural Fiore et al. [2003] Ozone, ppbv

8. LARGE DIFFERENCES BETWEEN MODELS IN GLOBAL TROPOSPHERIC OZONE PRODUCTION STE Tg yr -1 P Tg yr -1 L Tg yr -1 Dep Tg yr -1 Burden Tg Lifetime days IPCC TAR Wang98 770 ± 400 400 3420± 770 4100 3470± 520 3680 770± 180 820 300 ± 30 310 24 ± 2 25 IPCC 4AR GEOS-Chem 520± 100 470 4570± 680 4900 4150± 550 4300 1020± 220 1070 330 ± 30 320 25± 4 22 ACCENT GEOS-Chem GMI 520± 200 510 540-560 5060± 570 4490 4720-5330 4560± 720 3770 4400-5060 1010± 220 1020 760-860 340± 40 290 370-390 22± 2 22 24-26 Wu et al. (2006) GEOS-Chem 3 met fields 510-5404250-47003710-41301000-1090300-32021-23 Wu et al. [2006] 2/3 of variance in P(O x ) across models explainable by NO x emission, STE, and inclusion of NMVOCs

9. AN EXAMPLE OF TRANSPACIFIC TRANSPORT OF ASIAN AEROSOL POLLUTION AS SEEN BY MODIS X10 18 [molecules cm -2 ] Heald et al. [2006]

10. P3B DATA over NW Pacific (30 – 45 o N, 120 – 140 o E) WET SCAVENGING OF ASIAN AEROSOLS DURING LIFTING TO THE FREE TROPOSPHERE Park et al. [2005] TRACE-P observations over NW Pacific (Feb-Mar 2001) and GEOS-Chem simulations Sulfate is most important exported anthropogenic aerosol in model

11. …BUT ELEVATED OC AEROSOL IS OBSERVED IN FREE TROPOSPHERIC ASIAN OUTFLOW – CONTRIBUTION TO INTERCONTINENTAL POLLUTION? ACE-Asia aircraft observations over Japan (spring 2001) Observed (Huebert) GEOS-Chem (Chung & Seinfeld) correlated with CO – but also a 1-3  g sm -3 background; implies large secondary source of OC in free troposphere missing from present models; OC dominates aerosol loading in free troposphere Observed (Russell) OC/sulfate ratio Heald et al. [2005]

12. IMPROVE Total sulfate ASIAN SULFATE ENHANCEMENT AT U.S. SITES GEOS-Chem Asian sulfate NW US: 0.18 μgm -3 NW US: 0.72 μgm -3 NW US: 0.60 μgm -3 NW US: 1.04 μgm -3 Heald et al. [2006] IMPROVE Total sulfate

13. MODEL vs OBSERVED VISIBILITY DEGRADATION AT IMPROVE SITES (2001) Park et al. [2006] 1 0 x1 o resolution

14. MODEL (RED) vs. OBSERVED (BLACK) VISIBILITY STATS AT IMPROVE SITES (2001) Park et al. [2006]

15. COMPARING CMAQ AND GEOS-Chem TRANSPACIFIC POLLUTION: CMAQ ASIAN SULFATE ENHANCEMENT IN U.S. SURFACE AIR IS 5x GEOS-Chem, WHY? Concentration,  g m -3 Altitude, km Sulfate SO x TRACE-P P-3B Asian outflow observations (Mar-Apr 2001, <140 o E) Rokjin J. Park, in progress

16. COMPARISONS FOR AEROSOL NITRATE AND AMMONIUM: CMAQ-ICAP & GEOS-Chem vs. TRACE-P Concentration,  g m -3 Altitude, km Sulfate SO x Ammonium Nitrate Rokjin J. Park, in progress

17. CMAQ ASIAN OZONE ENHANCEMENT IN U.S. SURFACE AIR IS 0.5x GEOS-Chem, WHY? Concentration, pppbv Ozone CO NO y Rokjin J. Park, in progress Need to investigate CMAQ ozone underestimate in free troposphere – lightning? TRACE-P DC-8 Asian outflow observations (Mar-Apr 2001, <140 o E)

18. PLAN FOR GMI SIMULATIONS For a given GMI coupled aerosol-chemistry tropospheric configuration, conduct several 1-year sensitivity simulations with 2 o x2.5 o resolution: –Standard –Perturbed anthropogenic emissions …could zero out North American or global emissions as before; but wait for HTAP recommendations (they will likely want smaller perturbations) Archive high-resolution time series in U.S., Europe, Asia surface air, time series for aircraft missions Start with GMI 2001 simulation for comparison with GEOS-Chem, observations from TRACE-P, U.S. surface sites Conduct simulations with different GMI meteorological fields as available, same emissions and chemistry If resources allow, vary emissions and chemistry as well