A multi-model analysis of the tropospheric ozone budget David Stevenson 1, F.J. Dentener 2, M.G....
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Transcript of A multi-model analysis of the tropospheric ozone budget David Stevenson 1, F.J. Dentener 2, M.G....
A multi-model analysis of the
tropospheric ozone budgetDavid Stevenson1, F.J. Dentener2, M.G. Schultz3, K. Ellingsen4, T.P.C. van Noije5, O. Wild6,
G. Zeng7, M. Amann8, C.S. Atherton9, N. Bell10, D.J. Bergmann9, I. Bey11, T. Butler12, J. Cofala8, W.J. Collins13, R.G. Derwent14, R.M. Doherty1, J. Drevet11, H.J. Eskes5,
A.M. Fiore15, M. Gauss4, D.A. Hauglustaine16, L.W. Horowitz15, I.S.A. Isaksen4, M.C. Krol2, J.-F. Lamarque17, M.G. Lawrence12, V. Montanaro18, J.-F. Müller19, G. Pitari18,
M.J. Prather20, J.A. Pyle7, S. Rast3, J.M. Rodriguez21, M.G. Sanderson13, N.H. Savage7, D.T. Shindell10, S.E. Strahan21, K. Sudo6, and S. Szopa16
1. University of Edinburgh, School of GeoSciences, Edinburgh, United Kingdom. 2. Joint Research Centre, Institute for Environment and Sustainability, Ispra, Italy. 3. Max Planck Institute for Meteorology, Hamburg, Germany. 4. University of Oslo, Department of Geosciences, Oslo, Norway.
5. Royal Netherlands Meteorological Institute (KNMI), Atmospheric Composition Research, De Bilt, the Netherlands. 6. Frontier Research Center for Global Change, JAMSTEC, Yokohama, Japan. 7. University of Cambridge, Centre of Atmospheric Science, United Kingdom.
8. IIASA, International Institute for Applied Systems Analysis, Laxenburg, Austria. 9. Lawrence Livermore National Laboratory, Atmos. Science Div., Livermore, USA. 10. NASA-Goddard Institute for Space Studies, New York, USA. 11. Ecole Polytechnique Fédéral de Lausanne (EPFL), Switzerland.
12. Max Planck Institute for Chemistry, Mainz, Germany. 13. Met Office, Exeter, United Kingdom. 14. rdscientific, Newbury, UK. 15. NOAA GFDL, Princeton, NJ, USA. 16. Laboratoire des Sciences du Climat et de l'Environnement, Gif-sur-Yvette, France.
17. National Center of Atmospheric Research, Atmospheric Chemistry Division, Boulder, CO, USA. 18. Università L'Aquila, Dipartimento di Fisica, L'Aquila, Italy. 19. Belgian Institute for Space Aeronomy, Brussels, Belgium.
20. Department of Earth System Science, University of California, Irvine, USA 21. Goddard Earth Science & Technology Center (GEST), Maryland, Washington, DC, USA.
Tropospheric ozone budget• Ozone is an important greenhouse gas and air pollutant
• Ozone budget and lifetime crucial for:– Long-range transport– Global Warming Potentials– Oxidising capacity– Climate-Chemistry (radiative forcing and feedbacks)
• Previous intercomparisons (e.g. IPCC TAR literature survey) of modelled tropospheric ozone budget hampered by:– Definition of PO3 and LO3
– Definition of troposphere– Differences in emissions
• What we really want to understand are differences due to model formulation (chemistry, convection, resolution, mixing, boundary conditions…)
Defining the O3 or Ox budget
NO2 L: O3 + HO2
O3 + OHO(1D) + H2OO3 + alkenes
O3 deposition
O3O(3P) O(1D)
Stratospheric input
PAN
HNO3
HO2NO2
NO3
N2O5
dep
dep
NO
P: NO + RO2 + other net loss terms
Some studiesuse wider definition;should make only minor difference
Different model chemical schemes – potential source of differences
ACCENT Intercomparison
• Prescribed anthropogenic emissions– but modellers used their own natural emissions, so
still some emissions uncertainty
• Defined O3 budget terms– but some modellers used their own definitions,
specific to chemical scheme– requested 3D monthly mean P and L
– also O3 deposition; inferred stratospheric input
• Defined tropopause O3=150 ppbv– centralised analysis
20 Models supplied O3 budgets
• CHASER_CTM• CHASER_GCM• FRSGC/UCI• GEOS-CHEM• GMI/CCM3• GMI/DAO• GMI/GISS• LLNL-IMPACT• LMDz/INCA-CTM• LMDz/INCA-GCM
• MOZ2-GFDL• MOZART4• MOZECH• MOZECH2• STOCHEM-HadAM3• STOCHEM-HadGEM• TM4• TM5• ULAQ• UM_CAM
CTMs driven by analyses
CTMs driven by GCM outputCTMs coupled to GCMs
S1 Tropospheric O3 budget
-5000
50010001500200025003000350040004500500055006000650070007500
CH
AS
ER
_CT
M
CH
AS
ER
_GC
M
FR
SG
C
GE
OS
-CH
EM
GF
DL
GM
ICC
M
GM
IDA
O
gm
igis
LL
NL
-IM
PA
CT
LM
DzI
NC
A
LM
DzI
NC
Ac
MO
ZE
CH
NC
AR
ST
OC
HE
M_H
adA
M3
ST
OC
HE
M_H
adG
EM
TM
4
TM
5
UL
AQ
UM
_CA
M
Mea
n
Med
ian
Tg
O3/
yr
P L P-L D Sinf
Year 2000 Tropospheric O3 budget
Tg(O3)/yr P L D SinfB/Tg(O3) /days
ACCENT 5100 4670 1000 550 340 22IPCC TAR 3420 3470 770 770 300 24
Zonal Annual Mean Ozone chemical production
Relatively highvalues through
whole troposphere
Relatively lowvalues in
tropical UT
Differences at poles
Ozonechemical
productionmainly reflects
NOx distributions
Zonal Annual Mean Ozone chemical destruction
Ozonechemical
destructionmainly reflects
H2O distribution(also O3 distribution)
Zonal Annual Mean Ozone net chemical production
Surface level O3 Net Chemical Production
Multi-model ensemble mean ozone P, L, NCP
= 0.997 Surface
Ship NOx
Multi-model ensemble mean ozone P, L, NCP
= 0.975
Multi-model ensemble mean ozone P, L, NCP
= 0.930
Multi-model ensemble mean ozone P, L, NCP
= 0.870
Multi-model ensemble mean ozone P, L, NCP
= 0.792 Mid-tropnet destruction
Multi-model ensemble mean ozone P, L, NCP
= 0.700 Mid-tropnet destruction
Multi-model ensemble mean ozone P, L, NCP
= 0.600 Mid-tropnet destruction
Multi-model ensemble mean ozone P, L, NCP
= 0.505
Multi-model ensemble mean ozone P, L, NCP
= 0.422
Multi-model ensemble mean ozone P, L, NCP
= 0.355Upper-trop
net productionlightning
Multi-model ensemble mean ozone P, L, NCP
= 0.300Upper-trop
net productionlightning
Multi-model ensemble mean ozone P, L, NCP
= 0.250Upper-trop
net productionlightning
Multi-model ensemble mean ozone P, L, NCP
= 0.200Upper-trop
net productionlightning
Multi-model ensemble mean ozone P, L, NCP
= 0.150Upper-trop
net productionlightning
Multi-model ensemble mean ozone P, L, NCP
= 0.099Upper-trop
net productionlightning
Global O3 budget terms
O
3 lif
etim
e / d
ays
O3 burden / Tg(O3)
Results for asingle model,several scenarios
Colours signifydifferent models
Ensemble mean model (offset)
Higher burdengoes with
longer lifetime
Climate changeshortens lifetimebut burden canrise/fall
As emissions rise,burden increases,
lifetime falls
MFR
A2
Conclusions
• First well-constrained analysis of several model’s ozone budgets, with consistent definitions of budget terms, tropospheric domain, and anthropogenic emissions
• Broadly consistent gross features• Production reflects NOx distribution• Destruction reflects H2O (and O3) distribution• Some inter-model differences in lightning NOx/convection;
isoprene; H2O; polewards transport; BL• Quite large differences compared to IPCC TAR
– NOx and isoprene emissions– Stratospheric input
• Deposition also crucial; most of the O3 budget is in BL
Further information
• Dentener et al., in press, Env. Sci. Tech.– Overview of intercomparison
• Stevenson et al., in press, JGR– Tropospheric O3 and CH4
• Van Noije et al., in press, ACPD– NO2 columns, modelled & GOME
• Shindell et al., submitted, JGR– CO, modelled & MOPITT
• Dentener et al., submitted, GBC– Deposition of N and S
• Ellingsen et al., in prep.– Surface O3 air quality
• +probably more• [email protected]