randall martin space-based constraints on emission inventories of nitrogen oxides chris sioris,...
TRANSCRIPT
Randall Martin
Space-based Constraints on Emission Inventories of Nitrogen Oxides
Chris Sioris, Kelly Chance (Smithsonian Astrophysical Observatory)Chris Sioris, Kelly Chance (Smithsonian Astrophysical Observatory)Lyatt Jaeglé (Univerisity of Washington) Lyatt Jaeglé (Univerisity of Washington)
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, Indirect Effect, Nutrient DeliveryImplications for Tropospheric Ozone, Aerosols, Indirect Effect, Nutrient Delivery
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
Errorweightin
g
Conduct a Chemical Inversion & Combine Top-Down Conduct a Chemical Inversion & Combine Top-Down and Bottom-up Inventories with Error Weightingand Bottom-up Inventories with Error Weighting
A posteriori emissionsTop-Down Emissions
1015 molec cm-2
A Priori NOx EmissionsSCIAMACHY NO2 Columns
1011 molec N cm-2 s-1
GEOS-CHEM model
NO/NO2
W ALTITUDE
May-Oct 2004
48 Tg N yr-1
48 – 39 Tg N yr-1
A Posteriori Emission Inventory RevealsA Posteriori Emission Inventory RevealsMajor Discrepancy in NOx Emissions from MegacitiesMajor Discrepancy in NOx Emissions from Megacities
GEIA
r2=0.82 vs a priori
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
Large Change in NOx Emissions Near New York CityLarge Change in NOx Emissions Near New York City
1011 atoms N cm-2 s-1 1011 atoms N cm-2 s-1 1011 atoms N cm-2 s-1
A priori A posteriori A posteriori – A priori
8.3 Tg N 1.1 Tg N
r2 = 0.92
Evaluate Each Inventory By Conducting GEOS-CHEM Simulation & Evaluate Each Inventory By Conducting GEOS-CHEM Simulation & Sampling Model Along Aircraft Flight TracksSampling Model Along Aircraft Flight Tracks
NOx (ppbv)
Simulation with A Posteriori – Simulation with A Priori
HNO3 (ppbv)
7.2 Tg N
In Situ Airborne Measurements Support Top-Down In Situ Airborne Measurements Support Top-Down InventoryInventory
In Situ
GEOS-CHEM (A priori)
GEOS-CHEM (A posteriori)
New England New England + Gulf Remote
P-3 Measurements from Tom Ryerson (NOAA)
Speciated Inventory for Soil emissionsSpeciated Inventory for Soil 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
ConclusionsConclusions
• Growing confidence in top-down constraint on NOx emissions
• Gross-underestimate in NOx emissions from megacities
• Soil NOx emissions underestimated, especially from Northern Equatorial Africa
Funding:
• National Aeronautics and Space Administration (NASA)
• Canadian Foundation for Innovation (CFI)
• Nova Scotia Research and Innovation Trust (NSRIT)
• Natural Sciences and Engineering Research Council of Canada (NSERC)