1. Recent Advances in the Use of Chemical Transport Models in Atmospheric Chemistry Studies Greg Carmichael, University of Iowa

3. Models are an Integral Part of Atmospheric Chemistry Studies Flight planning Provide 4-Dimensional context of the observations Facilitate the integration of the different measurement platforms Evaluate processes (e.g., role of biomass burning, heterogeneous chemistry….) Evaluate emission estimates (bottom-up as well as top-down) New comprehensive data sets to test/evaluate models

4. TRACE-P/Ace-Asia EXECUTION Emissions -Fossil fuel -Biomass burning -Biosphere, dust Long-range transport from Europe, N. America, Africa ASIA PACIFIC Satellite data in near-real time: MOPITT TOMS SEAWIFS AVHRR LIS 3D chemical model forecasts: - x - GEOS-CHyEM - CFORS - z FLIGHT PLANNING Boundary layer chemical/aerosol processing ASIAN OUTFLOW Stratospheric intrusions PACIFIC

5. DC8P3  Two aircrafts – DC8 and P3 urban plumes  Chemical evolution during continental outflow, biomass burning, dust outbreaks, and urban plumes  22  22 flights out of Hong Kong, Okinawa and Tokyo  O 3, CO, SOx, NOx, HOx, RH and J  100m to 12000m China NASA GTE TRACE-P Mar’01- Apr’01

6. CFORS/STEM-2K1 Model Data Flow Chart Large-scale Meteorological Fields (JMA, NCEP, ECMWF CFORS/RAMS STEM-2K1 On-Line TUV wind velocities, temperature, pressure, water vapor content, cloud water content, rain water content and PV etc. Dust, Sea Salt, Lightning NO x Biogenic Emisisons Emission Preprocessor Biomass Emissions Volcanic SO 2 Emissions Anthropogenic Area Emissions Fuel/activity info Large Point Sources Satellite Observations (fire counts, ozone columns, sea surface temperature, etc.) Forecasts Or Post Analysis Tracers/Markers: SO2/SulfateDMS BCOC VolcanicMegacities CO fossilCO-Biomass EthaneEthene Sea SaltRadon Lightning NOx Dust 12 size bins

7. Ace-Asia & Trace-P Focused on Asian Outflow March 2, 2001 March 7, 2001 March 6, 2001 March 5, 2001 March 4, 2001 March 3, 2001 March 10, 2001 March 9, 2001 March 8, 2001

8. Fight Planning: Frontal outflow of biomass burning plumes E of Hong Kong Observed CO –Sacshe et al. Observed aerosol potassium - Weber et al. Biomass burning CO forecast Longitude 100 ppb

9. P-3B SO2 How Well Do Models Capture the Observed Features?

11. Predictability – as Measured by Correlation Coefficient Met Parameters are Best

12. Uncertainty analysis has revealed wide differences in our knowledge of the emissions of particular species in particular parts of Asia …

13. CO and some other species are sometimes systematically underpredicted … What does this tell us about the model – Model deficiency? Emissions problem?

14. Back Trajectories from High CO points. --- CO > 700 --- CO > 600 --- CO > 500 --- CO > 450 --- CO > 400

15. Back Trajectories from High CO point (Zoom & CO > 500 ppbv) --- CO > 700 --- CO > 600 --- CO > 500

16. 06GMT, April 07, 2001 06GMT, April 11, 2001 Ace Asia – Focus on Aerosols

17. April 9 April 12 Asian Outflow: Complex Mixture of Dust, Bio, and Fossil Components Data: Sugimoto, et al. Poster: A11A0060 Sataka et al.

19. Ron Brown observed high AOD in Japan Sea Takla makan Gobi Log10(Dust) AOD Observed Al and model dust Lidar Ext. Of Ron Brown = 0.2/km This may be Miyakejima sulfate Plate 2

20. BC SO4

21. BC at surfaceBC C-130 #11 April 19th What Do The Observations and Models Tell Us About Asian Emissions?

22. We ran back-trajectories from each 5 minute leg of merge data set, and kept track of each time a trajectory passed over a grid cell of the city and below 2 km. Classification of trajectory by the Source of Megacity. Age as determined by trajectory is also shown Before Big difference !!! We catch more number of fresh airmass from Shanghai and Seoul.

23. Comparing Modeled and Measured Ratios: We extracted all points associated with a specified city and calculated measured and modeled ratios.  BC/  CO This analysis suggests that there emissions may be related to an underestimation of a specific sector.

24. The Importance of Fossil, Biofuels and Open Burning Varies by Region -- Richness of Emissions Data Base Can be Exploited

25. Using Measurements and Model – We Estimate Contributions of Fossil, Biofuel and Open Burning Sources The Informatics Problem: Chemical Mass Balance Source Information Air Mass Markers Model Runs w/wo Source Sectors

26. How is Photochemistry Impacted By These Aerosols? 1) Photolysis Impacts

27. Surface reflection Ice cloud Water cloud EP/TOMS Total Ozone (Dobson) Dust Black Carbon Organic Carbon Sulfate Other PM2.5 and Other PM10 Sea Salt absorption by gas-phase species O 3, SO 2 and NO 2 Inputs from STEM 3-D field STEM TOP 15km O 3 (Dobson) below STEM top height TUV TOP 80km Overtop O 3 = Output: 30 kinds of J-values for SAPRC99 mechanism Framework for Analyzing Chemistry/Aerosol Interactions: Model (STEM+TUV) + Laboratory Studies + Field Experiment Heterogeneous rxns on dust for NO x, O 3, SO 2, HNO 3

28. Cloud Top Temperature (°C) Flight Altitude (m) A example: TRACE-P flights on March 27 DC-8 #15 P-3 #17 P-3 flight #17: volcanic plume observation DC-8 flight #15: frontal study DC-8 J[NO 2 ] P-3 J[NO 2 ]

29. Figure 13. Observed and simulated ozone concentrations under the three conditions along with the flight paths of P3 #17 from 2 to 4 GMT Aerosol Effects Dominate Ozone Formation Under This Case

30. How is Photochemistry Impacted By These Aerosols? 1) Photolysis Impacts

31. How is Photochemistry Impacted By These Aerosols? 2) Heterogeneous Rxns:Direct Ozone Loss? Dust BC Sulfate

32. Lessons Learned Asian outflow is complex, characterizing it requires 4-dimensional measurements. Impacts on chemistry and radiation appear to be important. Closer integration of emissions, models and measurements is necessary to better quantify our understanding of Asian aerosols.

33. Through a NSF ITR Grant we are developing data assimilation tools – we have a 3-d version ready for application

34. We are Developing General Software Tools to Facilitate the Close Integration of Measurements and Models The framework will provide tools for: 1) construction of the adjoint model; 2) handling large datasets; 3) checkpointing support; 4) optimization; 5) analysis of results; 6) remote access to data and computational resources.

37. We Have Now a Full 4d-VAR Version of STEM and are beginning to use it For Ace-Asia/Trace-P Analysis

38. Recent Papers Daescu, D., and G. Carmichael, An adjoint sensitivity method for the adaptive location of the observations in air quality modeling, Journal of the Atmospheric Sciences, Vol. 60, No. 2, 434-450 (2003) Damian, V., A. Sandu, M. Damian, F. Potra, and G. Carmichael, The Kinetic Preprosesor KPP – a Software Environment for Solving Chemical Kinetics, Computers & Chemical Engineering, 26, 1567-1579 (2002) Sandu, A., D. Daescu, and G. Carmichael, Direct and Adjoint Sensitivity Analysis of Chemical Kinetic Systems with KPP: Theory and Software Tools, Atmospheric Environment, in review, 2003

39. Thoughts on the Summer 2004 Experiments UI/CGRER Focus: Improving Forecasting and Analysis through Closer Integration of Observations and Models Flight Planning Air Quality Quick- look Post- Mission Test: Our ability to forecast 4-dimensional distributions of ozone and PM The utility of forecasts of ozone, fine particles in flight planning and quick-look analysis The utility of why-cast products (e.g., O 3 -production, VOC vs NO x limited regions, influence functions, hydrocarbon reactivity….) in flight planning and analysis and air quality forecasting Our ability to assimilate surface chemical observations into the forecasts; the impact of assimilation on the forecasts (for a sub-region; e.g., the NE) Targeted measurements that explore the concept of aircraft as “mobile super- sites” Forecasting Analysis

40. U. Iowa/Kyushu/Argonne/GFDL With support from NSF, NASA (ACMAP,GTE), NOAA, DOE