MOZART Development, Evaluation, and Applications at GFDL

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1 MOZART Development, Evaluation, and Applications at GFDL MOZART Users Meeting August 17, 25 Boulder, CO Arlene M. Fiore Larry W. Horowitz

2 Outline: MOZART Development, Evaluation, and Applications at GFDL Surface Ozone Bias over the United States - Comparison with observations (EPA AQS; CASTNet) - Sensitivity - Policy-relevant background Evaluation with 24 ICARTT observations * Vertically distributed biomass burning Trends (historical, future) in ozone and aerosols Methane control for climate and air quality CMDL CH 4 * *Special thanks to George Milly, the ICARTT Science Team, CMDL

3 MOZART-2 Comparison with AIRS: July p.m. Surface O 3 (ppbv) Mean Bias = 24±1 ppbv; r 2 =.5

4 Processes Contributing to Surface Ozone over North America Outside natural influences Long-range transport of pollution stratosphere lightning Lightning Background air Ocean Fires Land biosphere X Human activity NORTH AMERICA POLICY RELEVANT BACKGROUND (PRB) OZONE: Ozone concentrations that would exist in the absence of anthropogenic emissions from North America

5 Daily afternoon (1-5 p.m. mean) surface ozone from all CASTNet sites for March-October 21: PRB ozone over the U.S. is typically 2-35 ppbv PRB 26±7 ppbv GEOS-CHEM PRB 29±9 ppbv MOZART-2 CASTNet sites MOZART-2 Model GEOS-CHEM Model Both models predict consistent PRB range despite large surface O 3 bias in MOZART-2

6 MOZART-2 bias associated with domestic ozone production Background O Slope = -.14; intercept=25;r= North American O Slope =.81; intercept=33;r= MODEL OBSERVED Daily mean 1-5 p.m. June 1 Aug 31 at CASTNet stations

7 Substantial O 3 sensitivity to the uncertain fate (and yield) of organic isoprene nitrates High-NO x (very fast) NO RO NO OH 2 2 O 3 ISOPRENE Change in July mean 1-5 p.m. surface O 3 when isoprene nitrates (at 12% yield) act as a NO x sink Isoprene nitrates Sink for NO x? MOZART ppbv impact! ppbv Fiore et al., JGR, 25

8 -7 Change in eastern U.S. surface ozone bias due to sensitivity simulations Base case = simulation with isop. nitrates as a NO x sink MOZART-2 Base case +19 ppbv O 3 deposition velocities* Daytime PBL increased to 1 km PAN, NO 2 dep vels. = O 3 Including alkyl nitrate formation SYNOZ No isop. peroxide recycling Daytime PBL increased to 2 km 2 Xactive drydep/emis (not phot) Xactive phot/emis (not drydep) All Xactive; no clouds in phot MOZART-4 Fully Interactive Base case +21 ppbv

9 Outline: MOZART Development, Evaluation, and Applications at GFDL Surface Ozone Bias over the United States - Comparison with observations (EPA AQS; CASTNet) - Sensitivity - Policy-relevant background Evaluation with 24 ICARTT observations Vertically distributed biomass burning Trends (historical, future) in ozone and aerosols Methane control for climate and air quality CMDL CH 4 *

10 COMPARISON WITH ICARTT : Mean % Bias MOZART-4 (preliminary version) NCEP T62, 1999 NEI vs. All INTEX DC-8 observations June-Aug CO_UCIGC OZONE PAN HNO3_CIT CH4_UCIGC CH2O_NCAR CH2O_URI HCHO_GIT H2O2_URI H2O2_CIT HNO3_UNH CH3OOH_URI CO_MIXING_RATIO ISOPRENE ACETALDEHYDE ACETONE MEK NOX OH HO2 ETHANE PROPANE HO2NO2 %

11 Campaign Mean Vertical Profiles Model vs. INTEX DC-8 Observations OZONE (ppb) CO (ppb) H 2 O 2 _CIT (ppt) Altitude (km) NO x (ppt) PAN (ppt) HNO 3 _CIT (ppt)

12 Ozone Chemical Regime Model vs. INTEX DC-8 Observations (day; <2km; east of 1 W) HO 2 vs. NO 2 Model more HOx-rich (i.e., NO x -sensitive) and shows a stronger HO x -NO x correlation than observed.

13 Outline: MOZART Development, Evaluation, and Applications at GFDL Surface Ozone Bias over the United States - Comparison with observations (EPA AQS; CASTNet) - Sensitivity - Policy-relevant background Evaluation with 24 ICARTT observations Vertically distributed biomass burning Trends (historical, future) in ozone and aerosols Methane control for climate and air quality CMDL CH 4 *

14 Vertically Distributed Biomass Burning (BMB) Emissions 1. IPCC AR-4 BASE CASE (met year 2) -- monthly mean van der Werf emissions -- levels with tops at.1,.5, 1, 2, 3, and 6 km 2. ICARTT Summer daily emissions from Rynda Hudman & Solene Turquety, Harvard -- distributed up to 4 km, with 5% below 1 km

15 Change in SON composite max* CO concentrations (ppb) (Vertically distributed) (All at surface) 3 hpa 5 hpa 75 hpa 995 hpa increases just above the boundary layer decreases at surface and higher altitudes; interplay btw emissions and convection? *Composite max = daily max per grid point

16 Change in Tropospheric O 3 Columns (DU) Composite Seasonal Maxima* (Vertically distributed) - (All BMB emissions at surface) MAM SON JJA DJF Maximum impact ~1% near source region *Composite max = daily max per grid point

17 Outline: MOZART Development, Evaluation, and Applications at GFDL Surface Ozone Bias over the United States - Comparison with observations (EPA AQS; CASTNet) - Sensitivity - Policy-relevant background Evaluation with 24 ICARTT observations * Vertically distributed biomass burning Trends (historical, future) in ozone and aerosols Methane control for climate and air quality CMDL CH 4 *

18 Emission trends in MOZART-2 and resulting tropospheric burdens, used to drive GFDL climate model simulations for IPCC NOx Emissions NO x Emissions (Tg N) SO2 Emissions SO 2 Emissions (Tg SO 2 ) BC Emissions BC Emissions (Tg C) [Horowitz, in prep.] O3 Burden 8 SO4 Burden O 3 Burden (DU) SO 4 Burden (Tg S) BC Burden BC Burden (Tg C) Historical A2 A1B B1

19 Trends in Tropospheric O 3 Columns 186: Mean=24.1 DU 2: Mean= 34. DU A2 21: Mean 45.4 DU First step; next we ll examine climate impacts on chemistry with GFDL chemistry-climate model [Horowitz, in prep.]

20 Ozone Budgets in IPCC-AR4 from 19 Tropospheric Chemistry Models for Base Year 2 Ozone (Tg yr -1 ) X 19-Model Mean MOZART-2 MOZART-4 X MOZECH GEOS-CHEM Budgets from Stevenson et al., 25 PROD LOSS DEP STRAT Emissions for 2: EDGAR 3.2 GFED mean for biomass burning Scenarios for 23: Current Legislation (CLE) Maximum Feasible Reductions SRES A2 Climate change (CLE emissions)

21 Outline: MOZART Development, Evaluation, and Applications at GFDL Surface Ozone Bias over the United States - Comparison with observations (EPA AQS; CASTNet) - Sensitivity - Policy-relevant background Evaluation with 24 ICARTT observations Vertically distributed biomass burning Trends (historical, future) in ozone and aerosols Methane control for climate and air quality CMDL CH 4 *

22 MOZART-2 Methane Study Motivation: Methane controls benefit global air quality and climate by lowering background tropospheric O 3 Question: Are prior results from steady-state simulations with uniform, fixed CH 4 concentrations directly relevant to real-world emission controls? Approach: Multi-decadal transient simulations Reduce global anthrop. CH 4 emissions by 4%: (1) All in Asia (2) Everywhere in the globe (All simulations use T62 NCEP winds, recycled as needed)

23 Methane Emissions in EDGAR inventory: early 199s (Tg CH 4 yr -1 ) 24 Anthropogenic: Energy, landfills, wastewater Ruminants Rice 1 Total: 548 Based on values in the literature, we increased biogenic CH 4 emissions by 6 Tg Biomass Burning Ocean Biogenic

24 MODEL CH 4 CMDL CH 4 Seasonal cycle, inter-annual variability, increasing trend largely captured at remote sites Underestimates post-1998; indicating emissions increase?

25 MODEL CH 4 CMDL CH High Bias at high northern latitudes Inter-hemispheric gradient too high Low Bias at high southern latitudes Low bias at high southern latitudes

26 Transient simulations with EDGAR 199 emissions, beginning 199: (1) Standard (2) 4% decrease in global anthrop. emissions (18% of total CH 4 emissions) Methane (ppbv) Tg Ozone Global surface CH 4 conc. Standard -4% Anthrop. Emissions Decrease in Tropospheric O 3 Burden Difference (STD - GLOB4) Tg CO Decrease in global surface CH 4 conc. (standard 4% anth. emis. decrease Change in Methane Concentration (ppbv) Decrease in Tropospheric CO Burden Difference (STD - GLOB4)

27 CLIMATE IMPACTS: Change in July 2 Trop. O 3 Columns (to 2 hpa) 4% decrease in global anthrop. CH 4 emissions Zero CH 4 emissions from Asia (= 4% decrease in global anthrop.) No Asia (4% global decrease) Dobson Units Tropospheric O 3 column response is independent of CH 4 emission location except for small (~1%) local changes DU

28 U.S. Surface Afternoon Ozone Response in Summer also independent of methane emission location MEAN DIFFERENCE NO ASIAN CH 4 MAX DIFFERENCE (Composite max daily afternoon mean JJA) GLOBAL 4% DECREASE IN ANTHROP. CH 4 Stronger sensitivity in NO x -saturated regions (Los Angeles), partially due to local ozone production from methane

29 Summary: MOZART Development, Evaluation, and Applications at GFDL Surface Ozone Bias over the United States Typically 15-2 ppbv; sensitive to local chemistry Evaluation with 24 ICARTT observations Generally good; many species too high in boundary layer Vertically distributed biomass burning Small mean effect, up to ~1% episodically Trends (historical, future) in ozone and aerosols Past increases, future increases under some scenarios First step towards studying chemistry-climate interactions MOZART-2 near ensemble mean in IPCC 23 comparisons Methane control for climate and air quality Good agreement btw transient runs and remote surface obs. Nearing steady-state after 3 years (~3 e-folding lifetimes) 4% anthrop. CH 4 decrease -9 Tg O 3 ; -(1-3) ppbv U.S. JJA Ozone response largely independent of CH 4 source location

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