Improving emissions inventories in North America through systematic analysis of model performance during ICARTT and MILAGRO
During 2004 and 2006 the University of Iowa provided air quality forecast support for flight planning of the ICARTT and MILAGRO field campaigns. A method for improvement of model performance in comparison to observations is showed. The method allows identifying sources of model error from boundary conditions and emissions inventories. Simultaneous analysis of horizontal interpolation of model error and error covariance showed that error in ozone modeling is highly correlated to the error of its precursors, and that there is geographical correlation also. During ICARTT ozone modeling error was improved by updating from the National Emissions Inventory from 1999 and 2001, and furthermore by updating large point source emissions from continuous monitoring data. Further improvements were achieved by reducing area emissions of NOx y 60% for states in the Southeast United States. Ozone error was highly correlated to NOy error during this campaign. Also ozone production in the United States was most sensitive to NOx emissions. During MILAGRO model performance in terms of correlation coefficients was higher, but model error in ozone modeling was high due overestimation of NOx and VOC emissions in Mexico City during forecasting. Large model improvements were shown by decreasing NOx emissions in Mexico City by 50% and VOC by 60%. Recurring ozone error is spatially correlated to CO and NOy error. Sensitivity studies show that Mexico City aerosol can reduce regional photolysis rates by 40% and ozone formation by 5-10%. Mexico City emissions can enhance NOy and O3 concentrations over the Gulf of Mexico in up to 10-20%. Mexico City emissions can convert regional ozone production regimes from VOC to NOx limited. A method of interpolation of observations along flight tracks is shown, which can be used to infer on the direction of outflow plumes. The use of ratios such as O3/NOy and NOx/NOy can be used to provide information on chemical characteristics of the plume, such as age, and ozone production regime. Interpolated MTBE observations can be used as a tracer of urban mobile source emissions. Finally procedures for estimating and gridding emissions inventories in Brazil and Mexico are presented.
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