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