Hemispheric transport of ozone pollution and the nonlinearities
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Hemispheric transport of ozone pollution and the nonlinearities
GMI meeting
UC Irvine
March 17, 2008
Shiliang Wu, Harvard
Bryan Duncan, NASA / GSFC
Arlene Fiore, NOAA / GFDL
Daniel Jacob, Harvard
Oliver Wild, University of Lancaster
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HTAP Multi-model approach to estimate intercontinental source-receptor (S-R) relationships for ozone
20% decreases in:
anthrop. emis. in HTAP regions for NOx, CO, NMVOC individually
anthrop. emis. of all O3 and aerosol precursors in HTAP regions
global CH4
Conduct base simulations with 3-D models horizontal resolution of 4°x5° or finer 2001 meteorology each group’s best estimate for emissions in 2001 methane set to a uniform value of 1760 ppb
Conduct sensitivity simulations (17 total)
NA EUSA
EA
(Slide from Arlene Fiore @ GFDL)
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Estimates of S-R relationships: Springtime surface O3 decrease in HTAP receptor regions from 20% reductions of O3 precursors
0
0.20.4
0.6
0.8
11.2
1.4
NOx VOC CO ALL
EU and NA ≥ SA
RECEPTOR = EAST ASIA
20% foreign emis.) -20% domestic emis. ≈ 85%
pp
bv
EA/EU contribute similarly
EU VOC at least as important as NOx
RECEPTOR = NORTH AMERICA
pp
bv
20% foreign emis.) -20% domestic emis. ≈ 55%
SOURCE REGIONS: 3 foreign regions
0
0.2
0.4
0.60.8
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1.2
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NOx VOC CO ALL
Larger uncertainty in role of foreign VOC
(Slide from Arlene Fiore @ GFDL)
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Some questions remaining
Why so large variations across models associated with the role of VOCs?
Can 20% emission perturbations be scaled to other magnitudes? (Do the perturbations show good linearity? – this could have implications for the relative importance of different precursors in impacting the regional ozone export)
Do different models have similar/consistent linearity/nonlinearity for various perturbations?
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Large variations in EU AVOC inventories across models lead to large variations in calculated ozone export from EU
y = 0.0028x + 0.0362
R2 = 0.5898
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0.15
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0 5 10 15 20 25 30 35 40 45 50
EU AVOC inventories (Tg C / yr)
An
nu
al m
ea
n s
urf
ac
e O
3 d
ec
rea
se
s o
ve
r N
A (
pp
b)
GMI
GEOS-Chem
Annual mean NA surface O3 decreases (ppb) in response to 20% EU anthro. NMVOC reductions in different models
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Changes in surface O3 due to changes in EU AVOC emissions(simulation results from GMI model for JJA)
EU AVOC -20%
Full perturb / (20% perturb x 5)EU AVOC = 0
Control (ppb)
VOC perturbations are strongly linear
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VOC perturbations show very good linearity for all seasons
-0.5
-0.45
-0.4
-0.35
-0.3
-0.25
-0.2
-0.15
-0.1
-0.05
0
JAN FEB MAR APR MAY JUN JUL AUG SEP OCT NOV DEC
pe
rtu
rba
tio
ns
in O
3 (
pp
b)
(EU AVOC -20%) x 5
EU AVOC -100%
Changes in surface O3 over North America due to perturbations in EU anthro. VOC emissions (GMI results)
How about NOx?
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Changes in surface O3 due to changes in EA NOx emissions (simulation results from GMI model for JJA)
EA NOx -20%
Full perturb / (20% perturb x 5)EA NOx = 0
Control (ppb)
NOx perturbations show non-linearity
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Sensitivity to NOx emissions for different intercontinental pairsEA --> EUEA --> NA
-2
-1.6
-1.2
-0.8
-0.4
0
JAN FEB MAR APR MAY JUN JUL AUG SEP OCT NOV DEC
per
turb
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ns
in O
3 (p
pb
)
EU --> EAEU --> NA
-2
-1.6
-1.2
-0.8
-0.4
0
JAN FEB MAR APR MAY JUN JUL AUG SEP OCT NOV DEC
pe
rtu
rba
tio
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in O
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pp
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NA --> EANA --> EU
-4
-3
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-1
0
JAN FEB MAR APR MAY JUN JUL AUG SEP OCT NOV DEC
pe
rtu
rba
tio
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in O
3 (
pp
b)
- - - - (effects from -20% NOx) x 5 effects from -100%NOx
The nonlinearities for NOx perturbations are even larger for other seasons.
Distinctive seasonal pattern for the North America impacts on Europe?
Source region: EA
Source region: NA
Source region: EU
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Intercontinental influence on surface O3 for different precursors
Decrease in surface O3 (ppb) due to foreign emission reductions
0
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1
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20% reductions (HTAP models / MAM)
North America
Europe East Asia
South Asia
Fiore et al. [2008]Sensitivity to VOC comparable to NOx
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VOC
NOx
100% reductions (GMI/MAM)
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1
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VOC
NOx
North America
Europe East Asia
100% reductions (GMI/JJA)
Much weaker sensitivity to
VOC compared to NOx with full reductions or in
summer
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Intercontinental influence on surface O3 for different regions
Fiore et al. [2008]
-4
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JAN FEB MAR APR MAY JUN JUL AUG SEP OCT NOV DEC
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in O
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pb
)
(EU-20%)x5EU-100%(NA-20%)x5NA-100%
-3
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-2
-1.5
-1
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JAN FEB MAR APR MAY JUN JUL AUG SEP OCT NOV DEC
pe
rtu
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tio
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pp
b)
(EU-20%)x5
EU-100%
(EA-20%)x5
EA-100%
Foreign impact on NA (GMI)(HTAP)
(HTAP)
EU ~ EA?
NA ~ EU
Foreign impact on EA (GMI)
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Consistency and discrepancy across models(Changes in NA surface O3 due to changes in EU NOx emissions)
- - - ( perturbations from -20% EU anthro. NOx) x 5
__ perturbations from zeroing out EU anthro. NOx MZ = MOZART-v2 (from Arlene)FR = FRSGCUNI (from Oliver)
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MZ_SR3EU * 5 MZ_SR3zEU
FR_SR3EU * 5 FR_SR3zEU
GMI_SR3EU*5 GMI_SR3zEU
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- - - ( perturbations from -20% all EU anthro. emis) x 5
__ perturbations from zeroing out EU anthro. emis (NOx & VOC & aerosols)
Consistency and discrepancy across models(Changes in NA surface O3 due to changes in EU anthropogenic emissions)
-2.5
-2
-1.5
-1
-0.5
0
JUL AUG SEP OCT NOV DEC JAN FEB MAR APR MAY JUN
pe
rtu
rba
tio
ns
in O
3 (
pp
b)
MZ_SR6EU * 5MZ_SR6zEUFR_SR6EU * 5FR_SR6zEU
GMI_SR6EU*5GMI_SR6zEU
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On the family definition of Ox
Ox = O3 + O + NO2 + 2 NO3 + 3 N2O5 + PANs + HNO3 + HNO4
Ox = O3 + O + NO2 + 2 NO3 + 3 N2O5 + PANs + 2 HNO3 + HNO4 + other nitrates
Ox = O3 + O + NO2 + 2 NO3 + 3 N2O5 + PANs + 2 HNO3 + 2 HNO4 + HO2 + OH
…
Inconsistency in the family definition of Ox in literature on ozone budgets, leading to ambiguities in model intercomparisons.
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O3
O
NO2NO3 N2O5 HNO3
RNOx
HNO4
OH
HO2/RO2
HONO
H2O2/ROOH
Transport from stratosphere
Deposition
Carbonyls
Emission
h
12
Ox family
H2O, O2
A new family definition of Ox
(Slide from Daniel Jacob)
0.51
1.523
Ox = O3 + O + NO2 + 2 NO3 + 3 N2O5 +
PANs + 1.5 HNO3 + HNO4 + 0.5 HOy
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Thank you!