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Assessing the Parameterization of NOx Emissions By Lightning
in a Chemical Transport Model with HNO3 Columns from IASI
Matthew Cooper1
Randall Martin1,2, Catherine Wespes3,
Pierre-Francois Coheur3, Cathy Clerbaux3,4, Lee Murray5
1. Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia, Canada.2. Harvard-Smithsonian Center for Astrophysics, Cambridge, MA, USA3. Spectroscopie de l’Atmosphère, Chimie Quantique et Photophysique, Université Libre de Bruxelles, Brussels, Belgium4. Sorbonne Universités, UPMC Univ. Paris 06; Université Versailles St-Quentin; CNRS/INSU, LATMOS-IPSL, Paris, France5. NASA Goddard Institute for Space Studies and Lamont-Doherty Earth Observatory of Columbia University, NY, USA
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𝑁𝑂 𝑁𝑂2
𝐻𝑂2
𝑂3
𝐶𝑂
𝐻𝑁𝑂3
20-24 Tg
3-13 Tg
4-15 Tg
4-8 Tg
Global NOx Emissions Have Significant Uncertainty.Can Be Constrained Using HNO3 Observations.
𝑂𝐻
[Cooper et al., JGR 2014]
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IASI Satellite Provides Global HNO3 Columns.
IASI – A Nadir-viewing FTS
Global coverage 2x daily
Provides total column HNO3
Measurements over remote Pacific Ocean used alongside GEOS-Chem CTM to extract tropospheric portion of column
IASI Annual Mean Tropospheric HNO3 Column
[Cooper et al., JGR 2014]
IASI Annual Mean Total Atmospheric HNO3 Column
0 0.5 1.0 1.5 2.0 2.5 3(molec/cm2) x1020
0 0.5 1.0 1.5 2.0 2.5 3(molec/cm2) x1019
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GEOS-Chem HNO3 Lower Over Southeast Asia
IASI Annual Mean Tropospheric HNO3 Column
GEOS-Chem Annual Mean Tropospheric HNO3 Column
IASI – GEOS-Chem Percent Difference
mo
lec/
cm2
mo
lec/
cm2
Perc
ent
IASI: Nadir-viewing FTS Satellite instrument
GEOS-Chem: Global chemical transport model
GEOS-Chem too low, orIASI too high?
[Cooper et al., JGR 2014]
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Bias Due to Model Underestimating HNO3 in SE Asia
• Bias observed by multiple instruments, across large vertical region
[Cooper et al., JGR 2014]
* HIRDLS - Limb-viewing radiometer * ACE-FTS - Solar occulation FTS * Aircraft –PEM West B, PEM Tropics A campaigns *
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Lightning NOx is Most Likely Bias Source
•No error in CO gives confidence in anthropogenic and biomass burning emissions
•Deposition processes also ruled out via model studies
• Lightning emits NOx but not CO
[Cooper et al., JGR 2014]
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•GEOS-Chem lightning scaled by observed flash density
•SE Asia lightning flashes are longer, more radiant than elsewhere in tropics
• Intra-cloud lightning more common in SE Asia
[Beirle et al., Nat. Hazards Earth. System. Sci. Discuss, 2014]
Sim
ula
ted
IC/C
G F
lash
Rat
io
Some Regionally Varying Lightning Properties that could Affect SE Asia
[Cooper et al., JGR 2014]
Lightning Properties Observed by OTD/LIS
Simulated IC/GC Flash Ratio
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The GEOS-Chem Lightning Parameterization
Prescribed NOx/flash(260 mol/flash)
Flash rates match satellite observations
Prescribed vertical profiles
Emissions added
to GEOS-Chem
4°x5° grid boxes
[Cooper et al., JGR 2014]
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•Early subgrid plume has high NOx concentration
• Leads to rapid HNO3 production, lower OPE
• This is not represented in the model
LNOx Plumes have Sub-Grid Spatial Scale.LNOx Chemistry is Non-linear
Reality
In GEOS-Chem
[Kleinmann et al 2002]
(OP
E)
[Cooper et al., JGR 2014]
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A Simple LNOx Plume Pre-processor
GC Grid BoxNOx
HNO3 + 15O3
Current Mechanism With Pre-Processing
• Adding 0.5 Tg N to Southeast Asia gives better agreement
GC Grid Box
NOx
-1.0 -0.8 -0.6 -0.4 -0.2 0 0.2 0.4 0.6 0.8 1.0
HNO3 Tropospheric Column(IASI – Standard GEOS-Chem)/IASI (IASI – GC w/ PreProcessor)/IASI
92% Bias 6% Bias
[Cooper et al., JGR 2014]
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Conclusions
• Tropospheric HNO3 from IASI valuable for understanding NOx sources
• GEOS-Chem underestimates HNO3 in Southeast Asia
• Lightning NOx is most likely contributor to bias
• Developed representation of early stage of concentrated lightning NOx
plume
• A preprocessor for early stages of plume improves the simulation
[Cooper et al., JGR 2014]
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LNOx Plume Pre-processor VS
Prescribed Flash Yield
• Adding 0.5 Tg N to Southeast Asia gives better agreement
OzonesondeStandard3.5x Nox
Pre-Process
HNO3 Tropospheric Column(IASI – Standard GEOS-Chem)/IASI
(IASI –GEOS-Chem w/ Pre-Processor)/IASI