randall martin space-based constraints on emissions of nitrogen oxides with contributions from:...
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Randall Martin
Space-based Constraints on Emissions of Nitrogen Oxides
With contributions from:With contributions from:Chris Sioris, Kelly Chance (Smithsonian Astrophysical Observatory)Chris Sioris, Kelly Chance (Smithsonian Astrophysical Observatory)
Lyatt Jaeglé (Univerisity of Washington)Lyatt Jaeglé (Univerisity of Washington)Yongtao Hu, ArmisteadYongtao Hu, Armistead Russell (Georgia Tech) Russell (Georgia Tech)
Tom Ryerson (NOAA)Tom Ryerson (NOAA)
Relative Uncertainty
Global Surface NOGlobal Surface NOx x Emissions Uncertain to Factor of 2Emissions Uncertain to Factor of 2Implications for Tropospheric Ozone, Aerosols, and Indirect EffectImplications for Tropospheric Ozone, Aerosols, and Indirect Effect
Here in Tg N yr-1 (based on)Fossil Fuel 24 (GEIA)
Biomass Burning 6 (Duncan et al., 2003)
Soils 5 (Yienger and Levy, 1995)
NOx Emissions (Tg N yr-1)Fossil Fuel (20-33) Biomass Burning (3-13) Soils (4-21)
Top-Down Information from the GOME and Top-Down Information from the GOME and SCIAMACHY Satellite InstrumentsSCIAMACHY Satellite Instruments
•Nadir-viewing solar backscatter instruments including ultraviolet and visible wavelengths
• Low-elevation polar sun-synchronous orbit, late morning observation time
•GOME 1995-2002•Spatial resolution 320x40 km2
•Global coverage in 3 days
•SCIAMACHY 2002-presentSpatial resolution 60x30 km2
Global coverage in 6 days
Cloud-filtered Tropospheric NOCloud-filtered Tropospheric NO22 Columns Determined from SCIAMACHY Columns Determined from SCIAMACHY
May-Oct 2004
detectionlimit
Retrieval based on Martin et al., 2002, 2003
Retrieval:
Spectral fit
Remove stratosphere
Account for scattering
Use a CTM to Conduct a Chemical Inversion to Map NOUse a CTM to Conduct a Chemical Inversion to Map NOxx
Emissions from Retrieved NOEmissions from Retrieved NO22 Columns Columns
Emission
NO NO2
HNO3
lifetime ~hours
NITROGEN OXIDES (NOx)
BOUNDARYLAYER
GOMESCIAMACHY
NO/NO2
W ALTITUDE
Tropospheric NO2
column ~ ENOx
May-Oct 2004
48 Tg N yr-1
48 - 38 Tg N yr-1
Global Top-Down Emission Inventory RevealsGlobal Top-Down Emission Inventory RevealsMajor Discrepancy in NOx Emissions from MegacitiesMajor Discrepancy in NOx Emissions from Megacities
GEIA
ICARTT: COORDINATED ATMOSPHERIC CHEMISTRY CAMPAIGN OVER ICARTT: COORDINATED ATMOSPHERIC CHEMISTRY CAMPAIGN OVER EASTERN NORTH AMERICA AND NORTH ATLANTIC IN SUMMER 2004EASTERN NORTH AMERICA AND NORTH ATLANTIC IN SUMMER 2004
International, multi-agency collaboration targeted at regional air quality, pollution outflow, transatlantic transport, aerosol radiative forcing
Terra
ERS
MISR, MODIS, MOPITT
ERS-2
GOME
Envisat
SCIAMACHY
Aqua
AIRS, MODIS
NASA DC-8
UK BAE-143
DLR Falcon
NOAA-P3
Canada Convair
NASAProteus
North American NOx Emissions (May – October)North American NOx Emissions (May – October)Largest Change in Northeastern US CoastLargest Change in Northeastern US Coast
1011 atoms N cm-2 s-1 1011 atoms N cm-2 s-1 1011 atoms N cm-2 s-1
Bottom-up (NAPAP) Top-Down (SCIAMACHY) SCIAMACHY - NAPAP
7.6 Tg N 8.4 Tg N 0.8 Tg Nr2
= 0.85
Evaluate Top-Down and Bottom-Up NOx InventoriesEvaluate Top-Down and Bottom-Up NOx InventoriesConduct GEOS-CHEM Simulation For Each InventoryConduct GEOS-CHEM Simulation For Each Inventory
Sampled GEOS-CHEM Along Flight TracksSampled GEOS-CHEM Along Flight Tracks
NOx (ppbv)
Simulation with SCIAMACHY – Original NOx Emission Inventory
HNO3 (ppbv)
In Situ Airborne Measurements Support Top-Down In Situ Airborne Measurements Support Top-Down InventoryInventory
In Situ
GEOS-CHEM (Bottom-up)
GEOS-CHEM (Top-Down)
New England New England + Gulf Remote
P-3 Measurements from Tom Ryerson (NOAA)
Algorithm for partitioning top-down NOAlgorithm for partitioning top-down NOxx inventory (2000) inventory (2000)
Algorithm tested using synthetic retrieval
GOME NOx emissions
Fuel Combustion1. Spatial location of FF-dominated regions in a priori (>90%)1
Biomass Burning2. Spatiotemporal distribution of fires used to separate BB/soil
VIRS/ATSR fire countsSoils
No fires + background
2
Jaeglé et al., 2005
Soil emissionsSoil emissionsA posteriori 70% larger than a priori!
A prioriA priori A posterioriA posteriori
Largest soil emissions: seasonally dry tropical + fertilized cropland ecosystems
(±200%) (±90%)
r2 = 0.62
Soils
Onset of rainy season: Pulsing of soil NOx!
North Eq. Africa
Jaeglé et al., 2005
Soils
East Asia
Errorweightin
g
EMIS: Emissions Mapping Integration ScienceEMIS: Emissions Mapping Integration ScienceOptimize North American NOOptimize North American NOxx Emissions Emissions
A posteriori emissionsTop-Down Emissions
May-Oct 2004
1015 molecules cm-2
NOx Emissions (SMOKE/G.Tech)SCIAMACHY NO2 Columns
1011 molec N cm-2 s-1
Aug 2004