Critical Assessment of TOMS-derived Tropospheric Ozone: Comparisons with Other Measurements and Model Evaluation of Controlling Processes M. Newchurch.

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Critical Assessment of TOMS-derived Tropospheric Ozone: Comparisons with Other Measurements and Model Evaluation of Controlling Processes M. Newchurch 1, D. Sun 2, X. Liu 2, L. Emmons 3, L. Horowitz 4, J. H. Kim 5, D. Kinnison 3, G. Brasseur 6, D. Jacob 7, J. Logan 7, R.V. Martin 7, K. Han 5, S. Na 5 1. U. Alabama in Huntsville and NCAR/ACD, NSSTC 320 Sparkman Dr.,Huntsville, AL United States 2. U. Alabama in Huntsville NSSTC 320 Sparkman Dr., Huntsville, AL United States 3. NCAR/ACD, 1850 Table Mesa Dr., Boulder, CO United States 4. GFDL Princeton University, Princeton, NJ, United States 5. Pusan National University, Pusan, Korea, Korea, Republic of 6. Max Planck Insitiute for Meteorology and NCAR/ACD, Hamburg, Germany 7. Harvard University, Cambridge, MA, United States 3. Model Output of Tropospheric Ozone The MOZART calculation of tropospheric column ozone in 1997 (Figure 2) indicates a strong tropospheric ozone wave-1 feature. The tropospheric ozone maxima appear in north Africa over March and April and south Africa over June to November. There are maxima in Southern Africa and South America over June-November. High tropospheric ozone always occurs over the tropical continents and Atlantic Ocean, while low ozone occurs over the Pacific Ocean. The NOx emissions in this MOZART simulation were (in TgN/y): Industry 23.1, Biomass burning 8.7, Soils 6.6, lightning source 9, and aircraft emission source of The Harvard GEOS-CHEM simulation of tropospheric ozone in 1997 (Figures 3 and 4) differs in the magnitude of the maxima and minima and also in the magnitude of the spatial gradients compared to the MOZART calculation for The Tropical biomass burning season over Africa corresponds to the tropospheric ozone maximum. The peak in tropical west Pacific over September- December is a direct result of forest fires that occurred in Indonesia in The NOx emissions in this GEOS-CHEM simulation were (in TgN/y): fossil fuel combustion 23.1, biomass burning 6.1, soils 5.1, biofuels 2.2, aircraft 0.5, and 0.2 from the stratosphere. Figure 2. Monthly tropical tropospheric ozone calculated by MOZART-2 for (Lighting NOx = 9TgN/y) 6. Conclusion 5. Comparison with Ozonesonde Measurements Figure 8. Time series of the six indicated TOMS derivation methods compared to the ozonesonde observations at eight SHADOZ sites. Figure 3. Monthly tropical tropospheric ozone from GEOS over Dec 1996-Nov (Lighting NOx = 3 TgN/y) 4. Comparison of TOMS-based Methods and Model Output Figure 6. The difference between monthly CCP and GEOS-CHEM (CCP-GEOS: Nox=3Tg) tropospheric ozone in December 1996 – November Figure 5 indicates the difference between CCP and MOZART tropospheric ozone in Significant differences occur in the Atlantic and Africa areas, especially in North Africa. The difference between tropospheric ozone derived from CCP and the calculation of GEOS-CHEM in 1997 (Figure 6) ranges from -8DU to 4DU in most area. the largest difference occurs in the biomass burning season of northern Africa where the CCP does not show a tropospheric ozone enhancement. Another method (Scan-angle), however, does report this enhancement. Figure 7. The TOMS total ozone in December 1996 – November Figure 5. The difference between monthly CCP and MOZART (CCP-MOZART) tropospheric ozone in Figure 4. Monthly tropical tropospheric ozone from GEOS over Dec 1996-Nov (Lighting NOx = 6TgN/y) Figure 9. Monthly mean of ozonesonde observations at eight SHADOZ sites and model output from GEOS-CHEM (3 (blue) and 6(black) Tg NOx) and MOZART (2.5Tg NOx). The best evaluation metric for tropical tropo- spheric ozone is comparison to the SHADOZ ozonesonde observations ( nasa.gov/Data_services/shadoz/Shadoz_hmpg2. html). Although intra-station biases on the order of –5 to –10% with TOMS total column ozone exist, we adjust for these biases. After adjustment, the sonde comparisons to a variety of TOMS derivation methods results in the time series of Figure 8. At the Atlantic sites (left panels) both the sonde measurements and the satellite derivations are higher than their counterparts in the pacific Ocean sites (right panels). Inspecting the relationship between the various satellite derivations and the, presumably more accurate ozonesonde measurements, one sees that the satellite/sonde correspondence varies noticeably with station location. Current TOMS-based methods have significant method-to-method differences with a range of 10-20DU. Model results are sensitive to the NOx budget. The comparison of TOMS-based methods and model calculation indicates a significant difference in northern Africa. Monthly mean SHADOZ tropospheric ozone and model output are show in figure 9. Good consistency occurs at Fiji, Samoa, and Tahiti for both model results and rather good GEOS-CHEM (3 Tg NOx) comparison at all stations Introduction Due to the limited spatial coverage of ozonesonde measurements, Satellite techniques play an important role in deriving global tropospheric ozone. The various satellite retrieval methods, however, vary significantly in their derived values of tropospheric column ozone. We evaluate the correspondence between various satellite derivation techniques and model calculations of tropospheric ozone and also evaluate this correspondence in both the spatial and temporal morphology of ozone. 2. Six TOMS-based Methods Comparison There are several TOMS-based methods to derive tropospheric ozone. We examine five methods, CCP, CCD, TOR, SAGE/CCP, MR-TTO and Scan-angle. For example, in September 1997, the range of derived values differs by DU over significant areas of the globe (Figure 1), especially in heavy biomass burning areas, the method-to-method difference is larger. Those five methods report a similar tropospheric ozone structure: ozone enhanced in the Atlantic and low ozone in the Pacific, but the significant differences indicate the limited accuracy of these methods. Figure 1. Tropical tropospheric ozone column [DU] derived by six different methods along with the range at each location in September CCP results from Clear-cloudy Pairs of observations [Newchurch et al. 2000], CCD results from our calculation of the Convective Cloud Differential method prescribed by Ziemke et al. [1998], TOR results from our calculation of the Tropospheric Ozone Residual (TOMS-SAGE) prescribed by Fishman and Brackett [1997], SAGE-CCP results from a hybrid of the CCP and TOR methods, Modified Residual method by Thomson and Hudson [1999], and Scan-angle results from Kim et al. [2001].