1 Mike3/papers/tropoz/aguf98 12/2/98 16:30 1 Mike5/papers/presentations non ref/2002/Harvard 5/13/2002 Nsstc.uah.edu/atmchem Presented at Harvard University May 17, 2002 Mike Newchurc h Xiong Liu Da Sun Mohammed Ayoub University of Alabama in Huntsville Randall Martin Harvard University Jae Kim Pusan University, S. Korea Tropical Tropospheric Ozone from TOMS, Sondes, GOME, and Models: How well do we understand?

2 Mike3/papers/tropoz/aguf98 12/2/98 16:30 TOR Technique Tropospheric ozone the difference of TOMS total ozone and monthly averaged SAGE integrated stratospheric ozone. Fishman and Larsen, 1987.

3 Mike3/papers/tropoz/aguf98 12/2/98 16:30 CCD Technique (3) Stratospheric column ozone (as a function of latitude and time) is derived by averaging above-cloud column ozone amounts over the Pacific. ( (1) The high-reflectivity (R >0.9) cloud tops over the Pacific region usually lie near the tropopause. (2) Zonal (i.e., west to east) variability of stratospheric column ozone is negligible.

4 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Modified-Residual Technique Hudson and Thompson,

5 Mike3/papers/tropoz/aguf98 12/2/98 16:30 CCP Technique (1) Zonal wave structure of stratospheric ozone (2) R> 80%. (3) THIR-derived cloud- top pressure <200 mb (after adjustment). (4) if no THIR, Low-pass filter is applied to filter low-altitude clouds Newchurch et al., 2001

6 Mike3/papers/tropoz/aguf98 12/2/98 16:30 SAGE+CCP Method The method is the same to CCP technique, except that SAGE measurements are recognized as high- altitude cloudy points defined in CCP. The significant influence is the area with low occurrence frequency of high-altitude cloud, such as in the Atlantic Ocean and east Pacific Ocean.

7 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Scan-angle Technique (1) This is the normalized difference of TORE between that at nadir and high-scan positions as a function of altitude (2) The average kernel shows a broad response with its peak centered at 5-km altitude, suggesting that the diff of retrieved total ozone btw nadir and high scan angle can be used to derive trop ozone. Kim et al., JAS, 2001

8 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Other TOMS methods not studied here TOMS-MLS [Froidevaux, Chandra, Ziemke. TOMS-SBUV [Fishman and Balok, 1999]. Direct Fitting [Hudson and Frolov, in prep, 2002]. Cloud Slicing [Ziemke et al, 2001]. Topographic Contrast [Jiang and Yung, 1996; Kim and Newchurch, 1996; Kim and Newchurch 1998; Newchurch et al, 2001].

9 Mike3/papers/tropoz/aguf98 12/2/98 16:30

10 Mike3/papers/tropoz/aguf98 12/2/98 16:30 1. Original (20.8 DU) 2. Well-mixed (20.8 DU) 3. Homogeneous (20.8 DU) 4. Linearly increasing (20.8 DU) 5. Linearly decreasing (20.8 DU) 6. Upper 2 km (4.2 DU) 7. Lower 2 km (4.2 DU) ICOAEN is very dependent on ozone distribution in clouds. Ozone distributed in the upper part of cloud usually contributes more to ozone absorption in clouds.

11 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Radiative Transfer Errors Clouds: R% >= 80% Clear: R <= 20% Equatorial Africa [10  E, 5  S, 20  E, 2  S] [10  E, 2  N, 20  E, 5  N] Western Pacific Ocean [160  E, 5  S, 170  E, 2  S] [160  E, 2  N, 170  E, 5  N] Nimbus-7 Total Error in the Derived Tropospheric Ozone-16 DU-6 DU Contribution from calibration error*-7 DU-6 DU Contribution from cloud-height related errors**2 DU Contribution from retrieval efficiency ***-2 DU2 DU Contribution from other errors (mainly ozone absorption enhancement in clouds) **** -9 DU-4 DU Earth-Probe Total Error in the Derived Tropospheric Ozone-9 DU0 DU Contribution from calibration error*0 DU Contribution from cloud-height related errors**2 DU Contribution from retrieval efficiency ***-2 DU2 DU Contribution from other errors ****-9 DU-4 DU Table 1. Error Analysis in the Clear/Cloudy differences. Data used in this analysis include TOMS L2 data in 1980 and 1999, adjusted THIR in 1980, SHADOZ data in , Trace-A measurements at Brazzaville, Congo in The “true” tropospheric ozone results after correcting all the cloud-height related errors, ozone retrieval efficiency, calibration error, and ozone enhancement in clouds and unknown errors [Newchurch et al, 2001b]. * The assignment of calibration error to N7 only is based on cloud/clear total ozone difference. However, the total error in the derived tropospheric ozone will not change with this assignment. ** The errors are calculated for 1980 N7 TOMS data using the adjusted THIR data but are assumed the same in EP TOMS data. *** Error due to retrieval efficiency are calculated using TOMRAD and TOMSV7 algorithm with the SHADOZ and TRACE-A measurements as reference profiles. **** These errors are the remaining errors unexplained in the cloudy/clear total ozone difference.

12 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Tropospheric ozone from six satellite-based methods in Sep 1997 Surface/Boundary-Layer/Free

13 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Average Range of TTO from Six Methods Surface/Boundary-Layer/Free

14 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Mean Square Difference of CCD-MR Tropospheric Ozone Both assume flat stratosphere. Surface/Boundary-Layer/Free

15 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Mean Square Difference of CCP-CCD Tropospheric Ozone

16 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Adjustment to Ozonesonde data using SAGE stratospheric ozone Surface/Boundary-Layer/Free The difference between SHADOZ sonde total ozone and collated TOMS total ozone is ~2-10% in total ozone, varying with station. Left figure shows the scatter plot of TOMS total ozone and sonde total ozone without adjustment. Right figure show the same figure but the sonde total ozone is adjusted by the ratio of SAGE and sonde stratospheric ozone.

17 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Time series of 6 Methods and sondes Surface/Boundary-Layer/Free Time series of the six indicated TOMS derivation methods compared to the ozonesonde observations at four SHADOZ sites.

18 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Envelope of the 6 Methods and Sondes Surface/Boundary-Layer/Free Max and Min curves of the six indicated TOMS derivation methods compared to the ozonesonde observations at four SHADOZ sites

19 Mike3/papers/tropoz/aguf98 12/2/98 16:30 The Average Differences (SONDE - METHOD)  1 Standard Deviation and Standard Error of the Mean

20 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Scatter plots of 6 Methods and Ascension Island Sondes ( ) Blue #: slope Yellow #: offset Green #: correlation Coeff

21 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Scatter plots of 6 Methods and San Cristobal Sondes ( ) Blue #: slope Yellow #: offset Green #: correlation Coeff

22 Mike3/papers/tropoz/aguf98 12/2/98 16:30 MOZAIC ozone column at December 1987 and January 1991 are showed. The maximum flight height is at least 8Km. MOZAIC displays significantly more spatial sturcture than the monthly averaged TOMS CCP results. Comparison with MOZAIC Ozone Measurements

23 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Comparison to GOME Tropospheric ozone

24 Mike3/papers/tropoz/aguf98 12/2/98 16:30 GOME Tropospheric ozone in 1997 from RAL

25 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Model Output of Tropospheric Ozone Monthly tropical tropospheric ozone from GEOS-CHEM over Dec 1996-Nov (Lighting NOx = 3 TgN/y)

26 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Model Output of Tropospheric Ozone Monthly tropical tropospheric ozone from GEOS-CHEM over Dec 1996-Nov (Lighting NOx = 0 TgN/y)

27 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Model Output of Tropospheric Ozone Monthly tropical tropospheric ozone from GEOS-CHEM over Dec 1996-Nov 1997.(Lighting NOx = 6TgN/y)

28 Mike3/papers/tropoz/aguf98 12/2/98 16:30 The difference between monthly CCP and GEOS-CHEM (CCP - GEOS-CHEM: NOx=3Tg) tropospheric ozone in December 1996 – November Comparison of TOMS-based Methods and Model Output

29 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Comparison of TOMS-based Methods and Model Output The difference between monthly CCP and GEOS-CHEM (CCP - GEOS-CHEM: NOx=6Tg) tropospheric ozone in December 1996 – November 1997.

30 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Seasonal Tropospheric Ozone Model Calculation Marufu, L., F. Dentener, J. Lelieveld, M.O. Andreae, and G. Helas, Photochemistry of the African troposphere: Influence of biomass-burning emissions, J. Geophys. Res., 105, 14,513-14,530, 2000.

31 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Monthly mean of ozonesonde observations at eight SHADOZ sites and model output from GEOS-CHEM (3 (blue) and 6(black) Tg NOx) and sonde (red) Comparison with Ozonesonde Measurements

32 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Fire counts peak in 2000: North Africa: DJF South Africa and South America: JJA TTO Climatology from CCP ( ) Peak is at Sep- Oct “Tropical Atlantic Paradox” [Thomson 2000]

33 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Average Tropospheric Ozone at DJF for Six Methods

34 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Controlling Processes for “Tropical Atlantic Paradox” - Biomass Burning ozone precursors - Lightning NOx production - Dynamics: -Wind fields - Stratospheric Ozone intrusion into tropospheric ozone - Cross-equatorial transport of extra-tropical ozone

35 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Theoretical Basis for Taylor Diagrams Geometric relationship between the correlation coefficient R, the centered pattern RMS error E', and the standard deviations  f and  r of the test and reference fields, respectively [Taylor, 2001].

36 Mike3/papers/tropoz/aguf98 12/2/98 16:30 6 Methods compared to Ascension Sondes 1: CCP 2: CCD 3: TOR 4: SAGECCP 5: MR 6: SCAN Green circle is Ascension Sonde reference point. Concentric Blue arcs measure distance from TOMS method to sonde reference.

37 Mike3/papers/tropoz/aguf98 12/2/98 16:30 6 Methods compared to GEOS-CHEM in Central Pacific

38 Mike3/papers/tropoz/aguf98 12/2/98 16:30 SAGE+CCP Method 6 Methods compared to GEOS-CHEM in North Africa

39 Mike3/papers/tropoz/aguf98 12/2/98 16:30 6 Methods compared to GEOS-CHEM in South Atlantic

40 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Conclusions The range of TOMS-derived tropical tropospheric ozone (TTO) values exceeds 50% of the climatology in a significant fraction of seasons and locations. Significant spatial and temporal structure appears in the resulting ozone differences of techniques. This range, however, brackets the ozonesonde TTO values. Although the average bias TOMS/Sonde bias is < 5%, the slopes and correlations vary considerably from method to method and station to station. Taylor diagrams quantify the agreement between methods, sondes, and model. Radiative transfer simplifications induce potential errors in TOMS ozone columns over clouds on the order of 10 DU, which represents ~30% of the TTO. Model/TOMS differences exceed 20 DU (~<1/2 the TTO). All methods, except the scan-angle, differ with the model (and GOME) in wintertime N. Africa burning season (The N. Atlantic Paradox).

41 Mike3/papers/tropoz/aguf98 12/2/98 16:30 References Fishman, J., and A.E. Balok, Calculation of daily tropospheric ozone residuals using TOMS and empirically improved SBUV measurements: Application to an ozone pollution episode over the eastern United States, J. Geophys. Res., 104, 30,319-30,340, Fishman, J., and V.G. Brackett, The climatological distribution of tropospheric ozone derived from satellite measurements using version 7 Total Ozone Mapping Spectrometer and Stratospheric Aerosol and Gas Experiment data sets, J. Geophys. Res., 102, 19,275-19,278, Fishman, J., V.G. Brackett, E.V. Browell, and W.B. Grant, Tropospheric ozone derived from TOMS/SBUV measurements during TRACE A, J. Geophys. Res., 101, 24,069-24,069, Fishman, J., and J.C. Larsen, Distribution of total ozone and stratospheric ozone in the tropics: Implications for the distribution of tropospheric ozone, J. Geophys. Res., 92, , Hauglustaine, D., L. Emmons, M. Newchurch, G. Brasseur, T. Takao, K. Matsubara, J. Johnson, B. Ridley, J. Stith, and J. Dye, On the Role of Lightning NOx in the Formation of Tropospheric Ozone Plumes: A Global Model Perspective, J. Atmos. Chem., 38, , 2001.

42 Mike3/papers/tropoz/aguf98 12/2/98 16:30 References Hudson, R.D., and A.M. Thompson, Tropical tropospheric ozone from Total Ozone Mapping Spectrometer by a modified residual method, J. Geophys. Res., 103, 22,129-22,145, Jiang, Y., and Y.L. Yung, Concentrations of tropospheric ozone from 1979 to1992 over tropical Pacific South America from TOMS data, Science, 272, , Kim, J.H., and M.J. Newchurch, Climatology and trends of tropospheric ozone over the eastern Pacific Ocean: The influences of biomass burning and tropospheric dynamics, Geophys. Res. Lett., 23, , Kim, J.H., and M.J. Newchurch, Biomass-burning influence on tropospheric ozone over New Guinea and South America, J. Geophys. Res., 103, , Kim, J.H., M.J. Newchurch, and K. Han, Distribution of Tropical Tropospheric Ozone determined by the scan-angle method applied to TOMS measurements, J. Atmos. Sci., 58, , Newchurch, M.J., X. Liu, and J.H. Kim, Lower Tropospheric Ozone (LTO) derived from TOMS near mountainous regions, J. Geophys. Res., 106, 20,403-20,412, 2001a.

43 Mike3/papers/tropoz/aguf98 12/2/98 16:30 References Newchurch, M.J., X. Liu, J.H. Kim, and P.K. Bhartia, On the accuracy of TOMS retrievals over cloudy regions, J. Geophys. Res., 106, 32,315-32,326, 2001b. Newchurch, M.J., D. Sun, and J.H. Kim, Zonal wave-1 structure in TOMS tropical stratospheric ozone, Geophys. Res. Lett., 28, , 2001c. Newchurch, M. J., D. Sun, and J. H. Kim, Tropical tropospheric ozone derived using Clear-Cloudy Pairs (CCP) of TOMS measurements, submitted to J. Atmos. Sci., 2001d. Taylor, K.E., Summarizing multiple aspects of model performance in a single diagram, J. Geophys. Res., 106, , Ziemke, J.R., and S. Chandra, Seasonal and interannual variabilities in tropical tropospheric ozone, J. Geophys. Res., 104, 21,425-21,442, Ziemke, J.R., S. Chandra, and P.K. Bhartia, Two new methods for deriving tropospheric column ozone from TOMS measurements: Assimilated UARS MLS/HALOE and convective-cloud differential techniques, J. Geophys. Res., 103, 22,115-22,127, 1998.

44 Mike3/papers/tropoz/aguf98 12/2/98 16:30 References Ziemke, J.R., S. Chandra, and P.K. Bhartia, A new NASA data product: Tropospheric and stratospheric column ozone in the tropics derived from TOMS measurements, Bull. Am. Meteorol. Soc., 81, , Ziemke, J.R., S. Chandra, and P.K. Bhartia, "Cloud slicing": A new technique to derive upper tropospheric ozone from satellite measurements, J. Geophys. Res., 106, , Ziemke, J.R., S. Chandra, A.M. Thompson, and D.P. McNamara, Zonal asymmetries in southern hemisphere column ozone: Implications of biomass burning, J. Geophys. Res., 101, 14,421-14,427, 1996.

45 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Table. The Average Differences in (CCP - SHADOZ)  1 Standard Deviation (sd). The Adjusted Differences Resulted from Accounting for the TOMS Tropospheric Retrieval Efficiency by Using the Sonde Tropospheric Ozone Measurements. SHADOZ Sondes Scaled to SAGE/Sonde No Scale SHADOZ Station CCP- SHADOZ ±1sd Adj CCP- SHADOZ ±1sd CCP- SHADOZ ±1sd Adj CCP- SHADOZ ±1sd Ascension -6  5-3  3-3  4-1  2 San Cristobal 1  2-2  13  2-1  2 Natal -1  60  42  52  3 Nairobi -1  3-2  20  3-1  2 Java 3  6-1  44  60  4 Fiji 2  6-1  33  50  3 Samoa 5  51  37  42  2 Tahiti 4  61  46  52  3 Average 1  5-1  33  40  3

46 Mike3/papers/tropoz/aguf98 12/2/98 16:30 1 Nsstc.uah.edu/atmchem Regional Atmospheric Profiling Center for Discovery RAPCD Presented at Harvard Unversity May 17, 2000 Mike Mohammed Ayoub, Arastoo Biazar, David Bowdle, Sundar Christopher, Kirk Fuller, Noor Gillani, Quingyuah Han, Kevin Knupp, Xiong Liu, Dick McNider, Da Sun Atmospheric Science Department Earth System Science Center Jack Fix Collage of Science University of Alabama in Huntsville Maurice Jarzembski, Bill Lapenta NASA/MSFC/SD P K Bhartia, Tom McGee John Burris GSFC/Laboratory for Atmospheres Mike Hardesty/NOAA/ETL Vandana Srivastava/USRA

47 Mike3/papers/tropoz/aguf98 12/2/98 16:30 The RAPCD Vertical Distribution Science Questions Surface/Boundary-Layer/Free Troposphere/UT/LS Exchange 1.Can we accurately predict surface ozone and aerosol concentrations? 2.What are the vertical and long-range transport processes affecting local air quality? 3.Can we accurately calculate the power plant plume effect on air quality? 4.How are cloud processes, including lightning, different from clear-air processes for chemical effects? 5.What are the mechanisms responsible for nocturnal jet transport of Gulf-H 2 O- initiatiated convection? 6.What is the diurnal behavior of the boundary layer in the Tennessee valley?

48 Mike3/papers/tropoz/aguf98 12/2/98 16:30 The RAPCD Aerosol Science Questions Aerosol Optics and microphysics 1.What role does heterogeneous chemistry play in air quality? 2.What are the composition and optical properties of aerosols? 3.What is the effect of water uptake? 4.What is information content of RS measurements of aerosols? 5.What is the character of complex aerosols (organics, dust, soil, mixes)? 6. What are the roles of Biogenic Volatile Organic Compounds (BVOC) in ozone and aerosol production? 7.Cross-disciplinary studies: Biohazards, protemics, protonics.

49 Mike3/papers/tropoz/aguf98 12/2/98 16:30 The RAPCD Satellite Calibration/Validation Science Questions EOS Satellite calibration and validation 1.Provide ozone and aerosol profiles for cal/val of AIRS, TES, OMI, QuikTOMS, SAGE III, MLS, PICASSO-CENA, GOME, MISR. 2.What is the climatology and variability of the 3-D aerosol and ozone (and water vapor?) fields? 3.Validation of new Remote Sensing technology

50 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Boundary-layer Ozone and Aerosols Vertical cross sections of O 3 concentration and aerosol backscatter for the NW-SE flight legs passing over Nashville for the afternoon flights on July 12. Banta, R.M. et al., Daytime buildup and nighttime transport of urban ozone in the boundary layer during a stagnation episode, Journal of Geophysical Research, 17, 22,519-22,544, 1998.

51 Mike3/papers/tropoz/aguf98 12/2/98 16:30 (Without clutter panels min setup time) Mobile Integrated Profiler Configuration

52 Mike3/papers/tropoz/aguf98 12/2/98 16:30 MIPS RESEARCH GOALS Study evolution and structure of the stable NBL with particular focus on evolution and the processes associated with transient breakdowns in the inversion. Use a case study approach to address spatial variability in both the stable and unstable ABL. Corresponding mesoscale and LES modeling will further enhance our understanding of the NBL behavior.

GHCC/USWRP Satellite Assimilation Project FSL * Indicates regions of differential heating * Distinguishes clear/cloudy regions * Have high spatial and temporal resolution AVHRR Land Use GOES Skin Temperature GHCC Activities: Applications of Research: Develop and test GOES retrieval and assimilation algorithm for NWP models Assess quality of NESDIS products Provide model and satellite products to NWS and public via internet Insure transfer of research to operational community Operational Forecasting Regional-Scale Air Quality Studies Improved Understanding Of Land/Atmosphere Interactions The GOES Land Surface Data :

54 Mike3/papers/tropoz/aguf98 12/2/98 16:30 How well can we model the ozone variation? (July 4)(July 19)(July 24)(June29) TN LON: , LAT: 36.25

55 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Example of MSFC Ground-based Doppler Lidar

56 Mike3/papers/tropoz/aguf98 12/2/98 16:30 NPS: Annual average extinction coefficients (Mm -1 ) Huntsville, AL. A Researcher’s Paradise for Science of the Atmospheric Aerosol ‘Hot Topics’ in Aerosols and Forcing Chemical composition Speciation Hygroscopicity Physical properties Size distribution Morphology Radiometric Properties Extinction Scattering Absorption Polarimetric Forcing / Remote Sensing Optical depth Albedo Polarization Distribution of scattered light Vertical structure

57 Mike3/papers/tropoz/aguf98 12/2/98 16:30 NSSTC Regional Atmospheric Profiling Center for Discovery RAPCD Ozone Lidar Doppler Lidar Scanner Locked at zenith Grating Top Dome Floor Roof Top Dome Sidewall Railing Horizontal FTIR Solar FTIR Lid Closed Lid Open Dome Floor Chimney 2 Chimney 4 Chimney 5 Chimney 1 Dome Legs Dome Shutters Dome Chimney 3

58 Mike3/papers/tropoz/aguf98 12/2/98 16:30 Summary The Regional Atmospheric Profiling Center for Discovery, RAPCD, is designed to address atmospheric chemistry and air quality issues on the National agenda: –Processes controlling tropospheric trace gases and aerosols. –Aerosol characterization and effects. –Satellite calibration and validation. The constituency is broad: NASA, NSF, NOAA, EPA, DOE, State of Alabama. Co-Investigators comprise many NSSTC PIs in addition to several government laboratories and many instruments are already committed. This world-class laboratory facility will be ready July We are receiving interest from additional PIs to host their instruments. We invite interested investigators to join us.

59 Mike3/papers/tropoz/aguf98 12/2/98 16:30 nsstc.uah.edu/atmchem