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Frans Alkemade 1 , Michiel van Weele 1 , Peter van Velthoven 1 ,

Ability of global chemistry models to reproduce large scale UT/LS features of O3, CO, CH4 and acetone assessed by comparison to airborne CARIBIC data. Frans Alkemade 1 , Michiel van Weele 1 , Peter van Velthoven 1 , Sophie Szopa 2 , Thierry Elias 2 ,

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Frans Alkemade 1 , Michiel van Weele 1 , Peter van Velthoven 1 ,

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  1. Ability of global chemistry models to reproduce large scale UT/LS features of O3, CO, CH4 and acetone assessed by comparison to airborne CARIBIC data Frans Alkemade1, Michiel van Weele 1, Peter van Velthoven 1, Sophie Szopa 2, Thierry Elias 2, Andreas Zahn 4, Tanja Schuck 3, Carl Brenninkmeijer 3 and the CARIBIC team (1) KNMI, Royal Netherlands Meteorological Institute, de Bilt, the Netherlands (2) Laboratoire des Sciences du Climat et de l’Environnement, CEA/CNRS/UVSQ,IPSL, Gif-sur-Yvette, France (3) Max Planck Institute for Chemistry, Atmospheric Chemistry Division, Mainz, Germany (4) Institute for Meteorology and Climate Research, Forschungszentrum Karlsruhe, Karlsruhe, Germany Presentation: The Extra-tropical UTLS: observations, concepts and future directions Community workshop at NCAR, Boulder, CO October 21, 2009

  2. Focus / Questions / Goals • Can (our) models reproduce the observed large scale spatial and temporal variability and events? • How can we use CARIBIC to evaluate several aspects of the atmospheric chemistry models (transport+chemistry)? • Can we improve the models? • (NB: No CARIBIC data analysis  see presentation Andreas Zahn) F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  3. Overview - GEOMON: goal & means - CARIBIC: flights & data - TM5 : characteristics of model & emissions - LMDz-INCA : characteristics of model & emissions - Comparison CARIBIC observations to models (TM5 and LMDz INCA) , years 2005-2006 (flights 113 – 174, Southern destinations only) O3 CH4 (from October 2005 onwards) CO Acetone (case study for March 2006) - Conclusions & Future Plans F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  4. EU-GEOMON project (Global Earth Observation and Monitoring) Pilot study on measurements usage. Partners: KNMI, Un. Oslo, CEA Some Objectives : Demonstrate the usage of Geomon Greenhouse gas observations (CH4, CO2) for global model evaluation Use CARIBIC observations to evaluate model simulated large scale gradients in the upper troposphere/lower stratosphere Compare the model simulations to a climatology based on airborne measurements of CO2 and CH4 from ~45 different aircraft campaigns. F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  5. What is observed by Caribic? (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrumented Container) In Flight: H2Ogas H2Ocloud Ozone NO NOy (the sum of all reactive nitrogen species: NO, NO2, HNO3, PAN, N2O5, HNO2, HNO4, and nitrates) CO In flight remote sensing: BrO, HCHO, OClO, O4 WAS (Whole Air Sample ; 12 canisters, analyzed in laboratory) : CO2, CH4, N2O, SF6 (+ others) F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  6. CARIBIC flights F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  7. TM5 CTM some characteristics of model & emissions • 2 x 3 grid, 34 layers • ECMWF ERA Interim (EI) meteorology • O3 : Nudging to top boundary condition (climatology based on GOME / SCIA observations) • Emissions: selected datasets from GEMS and HYMN projects (see following slides) • Methane is fixed in the lowest two layers to a single value (1760.0 ppb). Stratospheric loss by OH F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  8. Anthropogenic emissionsfor GEOMON Ship and aircraft emissions: EC 6th FP IP Quantify Biomass burning emissions: GFEDv2 (van der Werf et al.) Other: year 2000 1x1 deg distributions IPCC/ACCENT; Remove ships and scale remainder with IIASA regional totals for 11 regions (‘MESSAGE’ land regions) For energy-related and non-energy related Year 2000 and scenarios for the years 2010, 2020,…2050 Linear interpolated emissions for the first decade: 2001,2002,…2009 Agricultural emissions from EDGAR (FT2000)

  9. Upscaling Asian CO emissions: Scaling factors wrt IPCC/ACCENT • increase of ~60% in China w.r.t IPCC/ACCENT (66 => 103 Tg) • Asia CO emissions now about half the global total of non-biomass burning anthropogenic CO Anthropogenic EDGAR, IIASA-scaled: 512 Tg(CO) Natural POET : 180 Tg(CO) Biomass burning GFEDv2 : 405 Tg(CO) Total for 2004: 1097 Tg(CO) F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  10. LMDz INCA (Laboratoire de Météorologie Dynamique - Interaction Chimie - Aérosols) characteristics of model & emissions • LMDz-INCA is a GCM, u and v are nudged on ECMWF-interim analysis (other dynamical fields being computed by LMDz • Emissions are those provided for the HYMN project (identical to those used by TM5) • The model considers the chemistry of methane and NMHC (89 tracers). • Stratospheric ozone is nudged to climate. • For CH4 no fixed surface value is used (unlike TM5), therefore a bias is to be expected, due to an equilibrium problem (a long run with sources=sink should be necessary to stabilize the model at the correct concentrations). The reference papers describing INCA are Hauglustaine et al. JGR 2004 and Folberth et al. ACP 2005. F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  11. Example of model evaluation: the CARIBIC flights of February 2006 (138-141)

  12. Reasonably good agreement for O3, CO, CH4 (Red = CARIBIC, Blue = TM5, Green = INCA) latitude altitude O3 CO CH4 Time 

  13. Correlations between O3, CO, CH4 latitude altitude O3 CO CH4

  14. Correlations between O3, CO, CH4 O3 O3 up,CO and CH4 down CO CH4

  15. These features correlate with PV anomaly  stratospheric intrusion Correlations:O3 up,CO and CH4 down

  16. Comparing Caribic – TM5 - LMDzINCA • Profiles and scatter plots of • O3 • CO • CH4 • CO- O3 scatter plots: identifying chemical transition from UT to LS • Acetone case study by LMDz INCA : 2006 flights #142-145 (Europe-South America). F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  17. Modelled vs Observed O3 Northern Hemisphere ( > 22) Model  TM5 INCA Observations  Dashed line: fit through all data Green line: data at locations where [O3] < 100 (troposphere) Blue line: data at locations where 100 < [O3] < 200 ( ~ UT/LS) Red line: data at locations where [O3] > 200 (stratosphere)

  18. O3 vertical distribution NH ( > 22) TM5 INCA Red: observations Blue: Model

  19. Scatter CH4 Northern Hemisphere ( > 22) Model  TM5 INCA Observations 

  20. CH4 vertical distribution (all data) TM5 INCA Red: observations Blue: Model

  21. CH4 vertical distribution NH ( > 22) INCA TM5 Red: observations Blue: Model

  22. CO Vertical distribution NH ( > 22) INCA TM5 Red: observations Blue: Model

  23. CO – O3 scatterplot : Modelled vs Observed Mixing Ratios Caribic Intrusion branche is missing INCA TM5

  24. Acetone Comparison LMDz-INCA / CARIBIC Branch of the acetone plume emitted by the Amazon forest #142 Why acetone ? Acetone modifies radical concentrations and then intervenes in atmospheric chemistry: impacts on ozone cycle, greenhouse warming. #145 #144 and #145 Map of daily average of acetone concentration modeled by LMDz-INCA for 21 March 2006, with superimposed airborne CARIBIC measurements. North Atlantic Ocean

  25. Future plans • Test use of OD (operational) meteo data instead of EI (ERA Interim reanalysed) meteo. • Improve upper boundary conditions (CH4, O3, CO) • Look at more tracers (NO, NOy, etc.) • More detailed assessment of GFED biomass burning and HYMN CH4 emissions. F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  26. Future: CH4 anthropogenic and natural emissions Anthropogenic Natural HYMN CH4 emissions Source Global Totals in 2004 (Tg CH4) Anthropogenic EDGAR, IIASA-scaled 293 Natural emissions LPJ-based 234 Biomass burning GFEDv2 vd Werff 20 Total emission 547 Soil sink LPJ-based -36 Net emission 511

  27. Conclusions • Variability / spread in the observations is not completely captured by models. ( problem with STE  better vertical model resolution needed in UT/LS) • However, large scale features are captured by both models. • Comparing the observed correlations of O3, CO and CH4 to the models can be used to assess the meteorological input fields. • Direct comparison between CARIBIC observations and models may help to assess the quality of emissions/processes and of the boundary conditions used by the models. F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  28. Thank you

  29. Some redundant slides follow F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  30. Anthropogenic NOX emissions: Similar as used in IPCC 4AR/ACCENT study (IIASA regionally rescaled) Anthropogenic EDGAR, IIASA-scaled 26.5 TgN Ship QUANTIFY 4.4 TgN Aircraft QUANTIFY 0.9 TgN Natural POET 8.0 TgN Biomass burning GFEDv2 5.3 TgN Lightning parameterised 5.4 TgN Total for 2004: 50.5 TgN

  31. LMDz INCA characteristics of model & emissions • LMDz-INCA is a GCM, u and v are nudged on ECMWF-interim analysis (other dynamical fields being computed by LMDzemissions are those provided for the HYMN project (the same than yours actually)It consider the chemistruy of methane and NMHC (89 tracers).We also nudged strato ozone on a climato.The reference papers describing INCA are Hauglustaine et al. JGR 2004 and Folberth et al. ACP 2005. F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  32.  The CEA is the French Atomic Energy Commission (Commissariat à l'énergie atomique) • *The National Institute of Sciences of the Universe**GEOMON is a scientific project within the 6th EU Framework Programme for Research and Development***The instruments and networks will be integrated into a larger system, which includes space missions and the development of digital tools to ensure all the measurements are compatible.****French laboratories involved in GEOMON: Laboratory of Climate and Environmental Sciences (IPSL/LSCE, a joint CEA, CNRS and Université Versailles Saint-Quentin laboratory), Aeronomics Service (IPSL/SA, a joint CNRS, Université Pierre et Marie Curie and Université Versailles Saint-Quentin laboratory), Laboratory of Dynamic Meteorology (IPSL/LMD, a joint CNRS, École polytechnique, Université Paris VI and ENS Paris laboratory), Inter-University Laboratory of Atmospheric Systems (LISA, a joint CNRS, Université Paris VII and Université Paris XII laboratory), the Laboratory of Atmospheric Optics (LOA, a joint Université Lille 1 and CNRS laboratory) and the Laboratory of the Atmosphere and Cyclones (LACy, a joint CNRS, Université La Réunion and Météo-France CNRM laboratory) F. Alkemade (KNMI): presentation at NCAR UTLS workshop, October 21st 2009

  33. Tropical mid-troposphere O3 (-22 22 latitude) Model  TM5 INCA Observations 

  34. Comparing O3 (all data 2005 - 2006) Model  TM5 INCA Observations  Dashed line: fit through all data Green line: data at locations where [O3] < 100 (troposphere) Blue line: data at locations where 100 < [O3] < 200 ( ~ UT/LS) Red line: data at locations where [O3] > 200 (stratosphere)

  35. [CH4] < 1700 ppb  must be stratospheric intrusion (otherwise, air would originate before 1990; implausible) TM5

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