Space-based Constraints on Emission Inventories of Nitrogen Oxides

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Space-based Constraints on Emission Inventories of Nitrogen Oxides Randall Martin Chris Sioris, Kelly Chance Space-based Constraints on Emission Inventories of Nitrogen Oxides Randall Martin Chris Sioris, Kelly Chance (Smithsonian Astrophysical Observatory) Lyatt Jaeglé (Univerisity of Washington) Tom Ryerson (NOAA)

Global Surface NOx Emissions Uncertain to Factor of 2 Implications for Tropospheric Ozone, Aerosols, Global Surface NOx Emissions Uncertain to Factor of 2 Implications 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) Relative Uncertainty

Top-Down Information from the GOME and SCIAMACHY Satellite Instruments • Nadir-viewing solar backscatter instruments Top-Down Information from the GOME and SCIAMACHY 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 320 x 40 km 2 • Global coverage in 3 days • SCIAMACHY 2002 -present Spatial resolution 60 x 30 km 2 Global coverage in 6 days

Cloud-filtered Tropospheric NO 2 Columns Determined from SCIAMACHY Retrieval: Spectral fit Remove stratosphere Account Cloud-filtered Tropospheric NO 2 Columns Determined from SCIAMACHY Retrieval: Spectral fit Remove stratosphere Account for scattering May-Oct 2004 detection limit Retrieval based on Martin et al. , 2002, 2003

Conduct a Chemical Inversion & Combine Top-Down and Bottom-up Inventories with Error Weighting A Conduct a Chemical Inversion & Combine Top-Down and Bottom-up Inventories with Error Weighting A Priori NOx Emissions SCIAMACHY NO 2 Columns NO/ NO 2 W ALTITUDE 1011 molec N cm-2 s-1 1015 molec cm-2 GEOS-CHEM model Top-Down Emissions Error weighting A posteriori emissions

A Posteriori Emission Inventory Reveals Major Discrepancy in NOx Emissions from Megacities 48 Tg A Posteriori Emission Inventory Reveals Major Discrepancy in NOx Emissions from Megacities 48 Tg N yr-1 May-Oct 2004 48 – 39 Tg N yr-1 GEIA r 2=0. 82 vs a priori

ICARTT: COORDINATED ATMOSPHERIC CHEMISTRY CAMPAIGN OVER EASTERN NORTH AMERICA AND NORTH ATLANTIC IN SUMMER ICARTT: COORDINATED ATMOSPHERIC CHEMISTRY CAMPAIGN OVER EASTERN NORTH AMERICA AND NORTH ATLANTIC IN SUMMER 2004 ERS-2 Envisat Terra Aqua GOME SCIAMACHY AIRS, MODIS MISR, MODIS, MOPITT NOAA-P 3 Canada Convair DLR Falcon NASA DC-8 NASA Proteus UK BAE-143 International, multi-agency collaboration targeted at regional air quality, pollution outflow, transatlantic transport, aerosol radiative forcing

Large Change in NOx Emissions Near New York City A priori r 2 = Large Change in NOx Emissions Near New York City A priori r 2 = 0. 92 7. 2 Tg N 1011 atoms N cm-2 s-1 A posteriori – A priori 8. 3 Tg N 1011 atoms N cm-2 s-1 1. 1 Tg N 1011 atoms N cm-2 s-1 Evaluate Each Inventory By Conducting GEOS-CHEM Simulation & Sampling Model Along Aircraft Flight Tracks Simulation with A Posteriori – Simulation with A Priori NOx (ppbv) HNO 3 (ppbv)

In Situ Airborne Measurements Support Top-Down Inventory New England + Gulf Remote GEOS-CHEM (A In Situ Airborne Measurements Support Top-Down Inventory New England + Gulf Remote GEOS-CHEM (A posteriori) In Situ GEOS-CHEM (A priori) P-3 Measurements from Tom Ryerson (NOAA)

Speciated Inventory for Soil emissions A posteriori 70% larger than a priori! A priori Speciated Inventory for Soil emissions A posteriori 70% larger than a priori! A priori (± 200%) A posteriori r 2 = 0. 62 (± 90%) Largest soil emissions: seasonally dry tropical + fertilized cropland e North Eq. Africa Soils Onset of rainy season: Pulsing of soil Jaeglé et al. , 2005

Conclusions • • • Growing confidence in top-down constraint on NOx emissions Gross-underestimate in Conclusions • • • 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)




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