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

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,

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

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

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)


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)

O3CH4 (from October 2005 onwards)COAcetone (case study for March 2006)

- Conclusions & Future Plans


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.


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)


CARIBIC flights

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


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 years2010, 2020,…2050

• Linear interpolated emissions for the first decade: 2001,2002,…2009

• Agricultural emissions from EDGAR (FT2000)


Upscaling Asian CO emissions:

Anthropogenic EDGAR, IIASA-scaled: 512 Tg(CO)Natural POET : 180 Tg(CO)Biomass burning GFEDv2 : 405 Tg(CO)

Total for 2004: 1097 Tg(CO)

• 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

Scaling factors wrt IPCC/ACCENT

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.


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

Reasonably good agreement for O3, CO, CH4(Red = CARIBIC, Blue = TM5, Green = INCA)

latitude

altitude

O3

CO

CH4

Time

Correlations between O3, CO, CH4

latitude

altitude

O3

CO

CH4

O3 up,CO and CH4 down

Correlations between O3, CO, CH4

O3

CO

CH4

Correlations:O3 up,CO and CH4 down

These features correlate with PV anomaly stratospheric intrusion

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).


Modelled vs Observed O3 Northern Hemisphere ( > 22)

Dashed line: fit through all dataGreen 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)

Observations

Model

TM5 INCA

O3 vertical distribution NH ( > 22)

TM5 INCA

Red: observationsBlue: Model

TM5 INCA

Observations

Model

Scatter CH4 Northern Hemisphere ( > 22)

CH4 vertical distribution (all data)

TM5 INCA


CH4 vertical distribution NH ( > 22)

TM5 INCA


CO Vertical distribution NH ( > 22)

TM5 INCA


Caribic

INCATM5

Intrusion branche is

missing

CO – O3 scatterplot : Modelled vs Observed Mixing Ratios

Acetone Comparison LMDz-INCA / CARIBIC

#142

#145

#144 and #145

Branch of the acetone plume emitted by the Amazon forest

North AtlanticOcean

Map of daily average of acetone concentration modeled by LMDz-INCA for 21 March 2006, with superimposed airborne CARIBIC measurements.

Why acetone ?Acetone modifies radical concentrations and then intervenes in atmospheric chemistry: impacts on ozone cycle, greenhouse warming.

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.


Future: CH4 anthropogenic and natural emissions

HYMN CH4 emissions Source Global Totals in 2004 (Tg CH4)

Anthropogenic EDGAR, IIASA-scaled 293Natural emissions LPJ-based 234Biomass burning GFEDv2 vd Werff 20Total emission 547Soil sink LPJ-based -36Net emission 511

Anthropogenic Natural

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.


Thank you

Some redundant slides follow


Anthropogenic NOX emissions:

Anthropogenic EDGAR, IIASA-scaled 26.5 TgNShip QUANTIFY 4.4 TgNAircraft QUANTIFY 0.9 TgNNatural POET 8.0 TgNBiomass burning GFEDv2 5.3 TgNLightning parameterised 5.4 TgNTotal for 2004: 50.5 TgN

Similar as used in IPCC 4AR/ACCENT study (IIASA regionally rescaled)

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.


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)


Tropical mid-troposphere O3 (-22 22 latitude)

Observations

Model

TM5 INCA

Comparing O3 (all data 2005 - 2006)

Observations

Dashed line: fit through all dataGreen 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)

TM5 INCAModel

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

TM5

Documents

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