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Intercontinental Source-Receptor Relationships for Ozone Pollution Arlene M. Fiore (arlene.fiore@noaa.gov) F. Dentener, O. Wild, C. Cuvelier, M. Schultz, C. Textor, M. Schulz, C. Atherton, D. Bergmann, I. Bey, G. Carmichael, R. Doherty, B. Duncan, G. Faluvegi, G. Folberth, M. Garcia Vivanco, M. Gauss, S. Gong, D. Hauglustaine, P. Hess, T. Holloway, L. Horowitz, I. Isaksen, D. Jacob, J. Jonson, J. Kaminski, T. Keating, A. Lupu, I. MacKenzie, E. Marmer, V. Montanaro, R. Park, K. Pringle, J. Pyle, M. Sanderson, S. Schroeder, D. Shindell, D. Stevenson, S. Szopa, R. Van Dingenen, P. Wind, G. Wojcik, J. West, S. Wu, G. Zeng, A. Zuber 40 th Air Pollution Workshop and Symposium, Raleigh, NC, April 7, 2008

Evidence of intercontinental transport at northern midlatitudes: 2001 Asian dust event Dust leaving the Asian coast in April 2001 Image c/o NASA SeaWiFS Project and ORBIMAGE Reduced Visibility from Transpacific Transport of Asian Dust Glen Canyon, Arizona Clear Day April 16, 2001

How do we estimate source-receptor (S-R) relationships that describe hemispheric transport of air pollution? 3D Model Structure Measurements at remote sites? (Monitoring site at Yosemite NP) Models with anthropogenic emissions reduced in source regions? Difficult to directly measure a region s contribution to pollution over a receptor region, particularly for ozone [e.g. Goldstein et al., 2004]

Regional control efforts (even under optimistic scenarios) may be offset by increases in hemispheric ozone pollution By 2030 under the Current LEgislation (CLE) scenario, the benefit of European emission control measures is significantly counterbalanced by increasing global O 3 levels [Szopa et al., GRL, 2006] U.S. grid-square days with 1-5p.m. O 3 > 70 ppb 1995 Base case 2030 A1 IPCC 2030 Scenario Anthrop. NO x emis. Global U.S. Methane emis. A1 +80% -20% +30% GEOS-Chem Model (4 x5 ) [Fiore et al., GRL, 2002] longer O 3 season U.S. air quality degrades despite domestic emissions controls (A1 2030) International approach to ozone abatement?

Convention on Long-Range Transboundary Air Pollution (CLRTAP) 51 parties in Europe, North America, and Central Asia Co-chairs: Terry Keating (U.S. EPA) and André Zuber (EC) TF HTAP Mission: Develop a fuller understanding of hemispheric transport of air pollution to inform future negotiations under CLRTAP

Multi-model assessment involving >25 modeling groups OBJECTIVES: Quantify S-R relationships for HTAP regions and assess uncertainties in these estimates NA HTAP S-R Regions EU SA EA Focus species: Ozone and precursors Aerosols and precursors Mercury Persistent Organic Pollutants Idealized Tracers Oxidized Nitrogen PRODUCTS: 2007 Interim Report to inform the review of the 1999 CLRTAP Gothenburg Protocol to abate acidification, eutrophication, and tropospheric ozone (www.htap.org). 2009 Assessment Report to inform the CLRTAP on hemispheric air pollution and S-R relationships.

Wide range in literature estimates of mean surface O 3 S-R relationships at northern mid-latitudes Receptor = North America Receptor = Asia Receptor = Europe Estimates are from studies cited in TF HTAP [2007] Ch5, plus new work [Holloway et al., 2008; Duncan et al., 2008; Lin et al., 2008] Assessment hindered by different: 1) methods 2) regional definitions 3) reported metrics 4) years (meteorology) Adopt a multi-model approach Consistency across models Examine all seasons A.M. Fiore

HTAP REGIONS A.M. Fiore Model Setup for TF HTAP Ozone S-R Study BASE SIMULATION horizontal resolution of 4 x5 or finer 2001 meteorology each group s best estimate for emissions in 2001 methane set to a uniform value of 1760 ppb SENSITIVITY SIMULATIONS (17 total) with sustained 20% decreases in regional anthrop. NO x, CO, NMVOC emis. individually (4x3) regional anthrop. emis. of all O 3 and aerosol precursors (4) global methane (to 1408 ppb) CASTNet EMEP EANET

Many models biased low at altitude, high over EUS+Japan in summer Good springtime/late fall simulation A.M. Fiore Large inter-model range; 21-model mean generally captures observed monthly mean surface O 3 Mediterranean Central Europe < 1km Central Europe > 1km Surface Ozone (ppb) NE USA SW USA SE USA Great Lakes USA Mountainous W USA Japan

Estimates of S-R relationships: Annual mean surface O 3 decrease from 20% reductions in anthropogenic NO x +CO+NMVOC emissions Source region: ppb 1.4 1.2 1 0.8 0.6 0.4 0.2 NA EU EA SA sum of 3 foreign regions Largest foreign S-R pair Similar impact from 3 foreign regions 0 Receptor region: NA EU E Asia S Asia Full range of 15 individual models NA EU SA EA Σ( 20% foreign anthrop. emis.) -20% domestic anthrop. emis. import sensitivity = 0.45-0.75 But seasonality in sensitivity to domestic vs. foreign sources? A.M. Fiore

A.M. Fiore Model ensemble mean surface O 3 response over NA to decreases in anthropogenic emissions of O 3 precursors -20% anthrop. NOx+CO+NMVOC emis. # models = 15, 17, 14, 14 # models = 15 Max influence in summer (NO x ) Max NMVOC contribution in winter Max foreign influence spring + late fall SA contributes least EU + EA contribute similarly Apr-Nov (but depends on model) Import Sensitivity for NA in July ~ 0.2, in April ~ 0.6

Model ensemble mean surface O 3 response over NA to decreases in anthropogenic emissions of O 3 precursors Foreign impact on NA (sum of O 3 responses to -20% anthrop. emis. in the 3 foreign regions) Model ensemble mean indicates a comparable influence from foreign NOx and NMVOC but relative importance varies across models Wide range in EU anthrop. NMVOC inventories used in the models large uncertainty in the estimated response of NA O 3 to EU emissions A.M. Fiore

Summary: Intercontinental S-R relationships for O 3 and conventional O 3 precursors Identified robust estimates + key areas of uncertainty Model ensemble mean overestimate vs. obs in summer EUS and Japan Robust: NA EU largest; SA others smallest Uncertainty in relative roles of EU/EA NA Uncertainty in exported EU O 3 from EU AVOC emissions inventories Import sensitivities in other regions? Comparison with prior literature?

A.M. Fiore Surface O 3 response to decreases in foreign anthropogenic emissions of O 3 precursors Robust conclusions: NA>EA>SA on EU ozone NA and EU often > SA or EA on each other; dominant contributor varies across models Ozone over foreign regions generally least sensitive to SA emissions Import sensitivities during month of max. domestic or foreign sensitivity: EU: 0.7 (APR) 0.3 (JUL) EA: 1.1 (MAR) 0.2 (JUL) SA: 0.5 (NOV)

A.M. Fiore Range of estimated S-R relationships narrows from that in the literature with consistently applied HTAP approach Assume linearity, scale response to -20% to 100% to estimate total contribution Receptor = NA Range in this work Range of published studies Model ensemble median Receptor = EU Receptor = EA

Summary: Intercontinental S-R relationships for O 3 and conventional O 3 precursors Identified robust estimates + key areas of uncertainty Uncertainty in exported EU O 3 from EU AVOC emissions inventories Robust: NA EU largest; SA others smallest Uncertainty in relative roles of EU/EA NA; EU/NA EA/SA Model ensemble mean overestimate vs. obs in summer EUS and Japan Estimated import sensitivities 0.2-0.3 July EA/NA/EU (max domestic production) 0.6-0.9 April EA/NA/EU (max foreign influence) 0.5 November SA (max foreign+domestic influence) Narrowed range of estimates from that in the literature How does role of CH 4 compare with NO x +CO+NMVOC?

Globally reducing methane decreases surface ozone everywhere Change in population-weighted mean 8-hr daily max surface O 3 in 3-month O 3 season (ppbv) Number of U.S. summer gridsquare days with O 3 > 80 ppbv 20% anth. NMVOC 20% anth. CO 20% anth. CH 4 20% anth. NO x Steady-state results from MOZART CTM West et al., GRL, 2007 1995 50% (base) anth. VOC 50% 50% 2030 anth. anth. A1 CH 4 NO x 2030 B1 GEOS-Chem results Fiore et al., GRL, 2002 Examine role of CH 4 vs. NO x +CO+NMVOC in multi-model context

A.M. Fiore Surface ozone decreases similarly in all HTAP regions when global methane is reduced 2 1.5 ppb 1 ANNUAL MEAN OZONE DECREASE FROM 20% DECREASE IN GLOBAL METHANE Full range of 18 individual models 0.5 0 Receptor: EU NA E Asia S Asia ~1 ppbv O 3 decrease over all NH receptor regions Consistent with prior studies Can we scale these results to 20% reductions in regional anthrop. CH 4 emissions to compare with conventional O 3 precursors?

Tropospheric O 3 responds approximately linearly to anthropogenic CH 4 emission changes across models + X MOZART-2 [this work] MOZART-2 [West et al., 2006,2007] TM3 [Dentener et al., 2005] GISS [Shindell et al., 2005] GEOS-CHEM [Fiore et al., 2002] IPCC TAR [Prather et al., 2001] Harvard [Wang and Jacob, 1998] Anthropogenic CH 4 contributes ~50 Tg (~15%) to tropospheric O 3 burden ~5 ppbv to surface O 3 Fiore et al., JGR, 2008

A.M. Fiore Comparable annual mean O 3 decrease from 20% reductions in foreign CH 4 emissions and NO x +NMVOC+CO Use CH 4 simulation + EDGAR 3.2 FT2000 CH 4 emissions [Olivier et al., 2005] to estimate O 3 response to -20% regional anthrop. CH 4 emissions 0.8 0.6 Sum of ozone decreases from 20% reductions in the 3 foreign regions ALL CH4 ppb 0.4 0.2 0 Receptor: NA EU E Asia S Asia

Conclusions: Intercontinental S-R Relationships for O 3 Identified robust estimates + key areas of uncertainty Model ensemble mean overestimate vs. obs in summer EUS and Japan Robust: NA EU largest; SA others smallest Uncertainty in relative roles of EU/EA NA Uncertainty in exported EU O 3 from EU AVOC emissions inventories Estimated import sensitivities 0.2-0.3 July EA/NA/EU (max domestic production) 0.6-0.9 April EA/NA/EU (max foreign influence) 0.5 November SA (max foreign+domestic influence) Narrowed range of estimates from that in the literature under HTAP setup Combined reductions in regional anthropogenic CH 4 + conventional O 3 precursors roughly double the O 3 decrease over foreign regions How might climate change affect hemispheric transport of air pollution? Are our S-R relationships consistent with rising Asian emissions driving a 0.1-0.5 ppb yr -1 surface O 3 increase (as derived from observations)?

Global background ozone may decrease in a warmer, more humid climate Mean annual change in number of days where daily max 8-hr O 3 > 80 ppbv (2090-2100 A1) (1990-2000) Less trans-pacific transport Increase in polluted (high-no x ) regions More inflow of clean air from Gulf of Mexico MOZART-2 global tropospheric chemistry model with meteorology from NCAR climate model [Murazaki and Hess, J. Geophys. Res., 2006] A.M. Fiore

Apply S-R relationships to address hypothesis of rising background O 3 driven by increasing Asian emissions OBSERVED: +0.1-0.5 ppb yr -1 in background surface O 3 [TF HTAP, 2007] Mace Head, Ireland SPACE-BASED NO 2 NO x EMISSIONS ASIA: +40% Simmonds et al., 2004 NA West Coast Richter et al., 2005 Assuming +10% yr -1 Asian emissions, our results imply an O 3 increase over NA and EU that falls at the low end of observed rise at the most OUR CAVEATS: Jaffe et al., 2003 -- assumes SA+EA, + other emissions follow NO x -- continental-avg vs. west coast obs Fig 3.6 from TF HTAP [2007] A.M. Fiore