Relationship Between NOx Emissions and NO2 Columns

1
Space-based Constraints on Emissions of Nitrogen
Oxides
Randall Martin
With contributions from Chris Sioris, Kelly
Chance (Smithsonian Astrophysical
Observatory) Lyatt Jaeglé (Univerisity of
Washington) Yongtao Hu, Armistead Russell
(Georgia Tech) Tom Ryerson (NOAA)
2
Global Surface NOx Emissions Uncertain to Factor
of 2Implications 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)

Relative Uncertainty
3
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 320x40 km2
• Global coverage in 3 days
• SCIAMACHY 2002-present
• Spatial resolution 60x30 km2
• Global coverage in 6 days

4
Cloud-filtered Tropospheric NO2 Columns
Determined from SCIAMACHY
Retrieval Spectral fit Remove stratosphere Accoun
t for scattering
May-Oct 2004
detection limit
Retrieval based on Martin et al., 2002, 2003
5
Use a CTM to Conduct a Chemical Inversion to Map
NOx Emissions from Retrieved NO2 Columns
GOME SCIAMACHY
Tropospheric NO2 column ENOx
BOUNDARY LAYER
NO2
NO
NO/NO2 ? ? W ALTITUDE
lifetime hours
HNO3
Emission
NITROGEN OXIDES (NOx)
6
Global Top-Down Emission Inventory RevealsMajor
Discrepancy in NOx Emissions from Megacities
48 Tg N yr-1
May-Oct 2004
48 - 38 Tg N yr-1
GEIA
7
ICARTT COORDINATED ATMOSPHERIC CHEMISTRY
CAMPAIGN OVER EASTERN NORTH AMERICA AND NORTH
ATLANTIC IN SUMMER 2004
ERS
ERS-2
Envisat
Terra
Aqua
SCIAMACHY
GOME
AIRS, MODIS
MISR, MODIS, MOPITT
NOAA-P3
Canada Convair
DLR Falcon
NASA DC-8
UK BAE-143
NASA Proteus
International, multi-agency collaboration
targeted at regional air quality, pollution
outflow, transatlantic transport, aerosol
radiative forcing
8
North American NOx Emissions (May
October)Largest Change in Northeastern US Coast
SCIAMACHY - NAPAP
Bottom-up (NAPAP)
Top-Down (SCIAMACHY)
1011 atoms N cm-2 s-1
1011 atoms N cm-2 s-1
1011 atoms N cm-2 s-1
r2 0.85
7.6 Tg N
0.8 Tg N
8.4 Tg N
9
Evaluate Top-Down and Bottom-Up NOx
InventoriesConduct GEOS-CHEM Simulation For Each
InventorySampled GEOS-CHEM Along Flight Tracks
Simulation with SCIAMACHY Original NOx Emission
Inventory
?HNO3 (ppbv)
?NOx (ppbv)
10
In Situ Airborne Measurements Support Top-Down
Inventory
New England
New England Gulf
Remote
GEOS-CHEM (Top-Down)
In Situ
GEOS-CHEM (Bottom-up)
P-3 Measurements from Tom Ryerson (NOAA)
11
Algorithm for partitioning top-down NOx inventory
(2000)
GOME NOx emissions
Algorithm tested using synthetic retrieval
Jaeglé et al., 2005
12
Soil emissions
A posteriori 70 larger than a priori!
A priori
A posteriori
r2 0.62
(90)
(200)
North Eq. Africa
East Asia
Soils
Soils
Onset of rainy season Pulsing of soil NOx!
Jaeglé et al., 2005
13
EMIS Emissions Mapping Integration
ScienceOptimize North American NOx Emissions
SCIAMACHY NO2 Columns
NOx Emissions (SMOKE/G.Tech)
Aug 2004
May-Oct 2004
1011 molec N cm-2 s-1
1015 molecules cm-2
Error weighting
A posteriori emissions
Top-Down Emissions