Thoughts on the Summer 2004 ExperimentsUI/CGRER Focus: Improving Forecasting and Analysis through Closer Integration of Observations and ModelsTest: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., O3-production, VOC vs NOx limited regions, influence functions, hydrocarbon reactivity.) in flight planning and analysis and air quality forecastingOur 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

Fine ChlorideFine SulfateTotal ExtinctionFine NitrateWe Plan to Forecast Size + Chemically Resolved Aerosol Products STEM simulations with on-line SCAPE compared to measurements of ACE-ASIA C-130 Flight 6Observations from PILS (Weber)

Impact of aerosols on photochemistry[Clarke][Avery]

A Scenario during TRACE-PIs value-added by forecasts of additional species?CONOxO3

STEM Forecast for ITCT2K2The locations with maximumO3 and CO may not be the same

Predicted sensitivity of O3 to VOCs and NOxVOC-limitedNOx-limited

Influence functions (over Cheju for O3 concentrations at 0:0:00 UT, 3/07/01) wrt O3, NO2, HCHO at -48, -24, -12 hr

Combining Back Trajectory and CMB Analysis to Estimate Contributions to Fossil, Biofuel and Open Biomass Burning to Airmasses2-D and 3-D analysis features for DC8 flight8 (March 9th)Left: same as previous figure, but (light blue: 3.4GMT, purple: 3.3GMT, red: 2.5GMT); Right: same as uppermost figure.Fly by animation

MOZART in ITCT 2K2Forecast modeDriven by NCEP AVN analysis + forecastRun at NCAR once daily, output every 6 hoursFull gas-phase O3 chemistry, regional tracersAnalysis modeRun after campaign, AVN analysis, higher res.O3 chemistry + tagged regional COOutput every 3 hours

Lessons from ITCT 2K2Importance of using timely met. forecastsComparison of chemical transport model forecastsIdentification of met. features associated with pollution / long-range transport

Examples from ITCT 2K2May 05 FlightLarge long-range transport (LRT) event (CO)May 10 FlightStratospheric intrusion (O3)

May 05 Flight, CO (ppbv)

May 05 Flight, CO (ppbv)

May 10 Flight, Ozone (ppbv)

May 10 Flight, Ozone (ppbv)

MOZART for ITCT 2K4Aerosol simulationSulfate, nitrate, ammonium, black carbon, organic carbon now includedMineral dust, sea salt being addedFull O3 photochemistry plus tagged CO speciesRun at ~2 deg resolution [driven by NCEP GFS ~ 0.5 deg]Run forecasts 4 times per day out to 84 hoursOutput every 3 hoursAutomated plots of forecast results posted to web siteCouple with regional model (STEM)

Issues for ITCT 2K4 (vs. 2K2)Long-range transport (LRT) less importantShould be easier for modelsBut, less lead timeEmission inventories should be more reliableMore emphasis on aerosolsWashout parameterizationTest understanding of organic aerosolsNighttime chemistry

Science Questions for ITCT 2K4TransportWhat other U.S. source regions impact pollutant levels in New England?What are the major export pathways during summer?Are these pathways well-simulated in models?Chemical transformationsCan we simulate the chemical evolution of air masses from source regions to the North Atlantic? (e.g., O3 production, NOy partitioning)AerosolsWhat is the composition of aerosols transported from North America to the North Atlantic?Are aerosol aging and removal processes well-simulated in models?What are the main sources of organic aerosols?

Development of a General Computational Framework for the Optimal Integration of Atmospheric Chemical Transport Models and Measurements Using Adjoints(NSF ITR/AP&IM 0205198 Started Fall 2002) A collaboration between:Greg Carmichael (Dept. of Chem. Eng., U. Iowa)Adrian Sandu (Dept. of Comp. Sci., Mich. Inst. Tech.)John Seinfeld (Dept. Chem. Eng., Cal. Tech.)Tad Anderson (Dept. Atmos. Sci., U. Washington)Peter Hess (Atmos. Chem., NCAR)Dacian Daescu (Inst. of Appl. Math., U. Minn.)

Goal: To develop general computational tools, and associated software, for assimilation of atmospheric chemical and optical measurements into chemical transport models (CTMs). These tools are to be developed so that users need not be experts in adjoint modeling and optimization theory.

Approach: Develop efficient algorithms for 4D-Var data assimilation in CTMs;

Develop software support tools for the construction of CTM adjoints;

Apply these techniques to: (a) analysis of emission control strategies; (b) integration of measurements and models to produce optimalanalysis data sets for field experiments; (c) inverse analyses to produce a better estimate of emissions;(d) design observation strategies to improve chemical forecasting

Iowa/GFDL/Argonne STEM Model DeploymentMesoscaleMeteorological Model(RAMS or MM5)MOZART Global Chemical Transport ModelSTEM Prediction Model with on-line TUV & SCAPEAnthropogenic & biomass burning EmissionsTOMS O3Chemistry & TransportAnalysisMeteorological Dependent Emissions(biogenic, dust, sea salt)STEM Tracer Model (classified tracers for regional and emission types)

STEM Data-Assimilation ModelObservationsAirmasses andtheir age & intensityAnalysisInfluence FunctionsEmission Biases

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

Thoughts on the Summer 2004 ExperimentsUI/CGRER Focus: Improving Forecasting and Analysis through Closer Integration of Observations and ModelsTest: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., O3-production, VOC vs NOx limited regions, influence functions, hydrocarbon reactivity.) in flight planning and analysis and air quality forecastingOur 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

We Plan to Look for Ways to Improve the Quality of the Emission Inventories by Close Integration with Modeling ActivitiesAnticipated Activities:Refine PM InventoriesRefine/Add species to aid in analysis (e.g., OCS, halocarbons, ethanol). We look for input on species of interest.Possible other activities: trends, consistent N-Hemisphere inventory, forecasts of emissions,

The BC problem

Surface reflectionIce cloud Water cloud EP/TOMS Ozone (Dobson)SCAPE AerosolEquilibriumModuleAerosolsabsorption by gas-phase species O3, SO2 and NO2Inputs from STEM 3-D field STEM TOP O3 (Dobson) below STEM top TUV TOP80kmOvertop O3 =Heterogeneous reactions on BC for NO2, O3, SO2, HNO3Outputs:

Aerosol composition (size-resolved),

Aerosol heterogeneous influences, J-values

STEM schematics for on-line TUV and on-line SCAPE

ITCT2K2 Post-Run with MOZART Boundary ConditionsTop and Lateral Boundary Conditions from MOZART II every 3 hoursSTEM 80x70 domain13.4kmmapped species: O3, CO, ethane, ethene, propane, propene, ethyne, HCHO, CH3CHO, H2O2, PAN, MPAN, isoprene, NO, NO2, HNO3, HNO4, NO3, and MVK Lateral boundary conditions of other species, included SO2 and sulfate still come from the large-scale CFORS tracer model

May 05 Flight

May 10 Flight

Obs from PILS (R. Weber)J(NO2) ShetterO3 AveryAOE ClarkeLeft: same as uppermost figure, but (light blue: 3.4GMT, purple: 3.3GMT, red: 2.5GMT); Right: same as uppermost figure.