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Constraints on the Production of Nitric Oxide by

Lightning as Inferred from Satellite Observations

Randall Martin
Dalhousie University

With contributions from


Bastien Sauvage & Ian Folkins: Dalhousie Univeristy
Christopher Sioris: Environment Canada
Christopher Boone and Peter Bernath: University of Waterloo
Jerry Ziemke: NASA Goddard
Global Lightning NOx Source Remains Uncertain
Constrain with Top-down Satellite Observations

SCIAMACHY
Tropospheric NO2 Columns
ACE-FTS
Limb HNO3 in Upper Troposphere
OMI & MLS
Both instruments onboard Aura satellite
Tropospheric O3

Lightning: responsible for >35% of global OH & tropical tropospheric O 3


Sauvage et al., 2007
Current Estimate of Annual Global NOx Sources
As Used In GEOS-Chem

Lightning
Global: 6.0 Tg N yr-1
Tropics: 4.4 Tg N yr-1

Other NOx sources:


(fossil fuel, biofuel,
biomass burning,
soils)
39 Tg N yr-1

1010 molecules N cm-2 s-1


Tropospheric NO2 Columns Retrieved from SCIAMACHY

Nov - Apr

NO
/NO2  
w Altitude

May - Oct

Retrieval Uncertainty
±(5x1014 molec cm-2 + 30%)

Tropospheric NO2 (1015 molecules cm-2)


Data from Martin et al., 2006
Simplified Chemistry of Nitrogen Oxides
Exploit Longer Lifetimes in Upper Troposphere
Upper
hv Troposphere
NO NO2 Ozone (O3)
O3, RO2 lifetime ~ month

NOx lifetime ~ week


HNO3 lifetime ~ weeks

NO
/NO2  
with altitude
Boundary
hv
Layer
NO NO2 Ozone (O3)
O3, RO2 lifetime ~ days
NOx lifetime < day
HNO3

Nitrogen Oxides (NOx)


Strategy

1) Use GEOS-Chem model to identify species, regions, and time


periods dominated by the effects of lightning NOx production

2) Constrain lightning NOx source by interpreting satellite


observations in those regions and time periods
Simulated Monthly Contribution of Lightning, Soils, and
Biomass Burning to NO2 Column

Martin et al., 2007


Annual Mean NO2 Column at Locations & Months with >60%
from Lightning, <25% from Surface Sources
SCIAMACHY (Uses 15% of Tropical Observations)

Meridional Average

GEOS-Chem with Lightning


(6±2 Tg N yr-1)
SCIAMACHY
GEOS-Chem with Lightning (8% bias, r=0.75)

GEOS-Chem without Lightning (-60% bias)

GEOS-Chem without Lightning

NO2 Retrieval Error


~ 5x1014 molec cm-2
Tropospheric NO2 (1014 molec cm-2)
Martin et al., 2007
ACE HNO3 over 200-350 hPa for Mar 2004 – Feb 2006

HNO3 Mixing Ratio (pptv)


V2.2 reprocessed data
GEOS-Chem Calculation of Contribution of Lightning to HNO3

HNO3 With
Lightning Fraction of Focus on
(6±2 Tg N yr-1) HNO3 from 200-350 hPa
Lightning

No Lightning

HNO3 from Lightning Fraction from Lightning

Jan

Jul

Martin et al., 2007


Annual Mean HNO3 Over 200-350 hPa at Locations &
Months with > 60% of HNO3 from Lightning
ACE (Uses 72% of Tropical Measurements)
Meridional Average

GEOS-Chem with Lightning


(6±2 Tg N yr-1)
ACE-FTS v2.2
research ______
reprocessed - -
GEOS-Chem with Lightning (-6% bias, r=0.81)

GEOS-Chem without Lightning


GEOS-Chem without Lightning (-77% bias)

HNO3 Retrieval Error


~35 pptv

Martin et al., 2007


+reprocessed
HNO3 Mixing Ratio (pptv)
OMI/MLS Tropospheric Ozone Column

Jan

Jul

Data from Ziemke et al. (2006)


Calculated Monthly Contribution of Lightning to O3 Column

O3 Column from Lightning Column Fraction from Lightning

Martin et al., 2007


Annual Mean Tropospheric O3 Columns at Locations &
Months with > 40% of Column from Lightning
OMI/MLS (Uses 15% of Tropical Measurements)
Meridional Average

GEOS-Chem with Lightning


(6±2 Tg N yr-1)

GEOS-Chem with Lightning (-1% bias, r=0.85)

OMI/MLS

GEOS-Chem without Lightning (-45% bias) GEOS-Chem without Lightning

O3 Retrieval Error
< 5 Dobson Units
Tropospheric O3 (Dobson Units) Martin et al., 2007
Lightning NOx Dominant Source for Tropical Tropospheric Ozone
Sensitivity to decreasing NOx emissions by 1% for each source
DJF 6 Tg N/yr 6 Tg N/yr 6 Tg N/yr

MAM

JJA

SON

ΔDU

Lightning Ozone Production Efficiency = 3 times OPE of each surface source

Sauvage et al., 2007


Simulated Annual Mean Characteristics

O3 ppb NOx ppb

Injection of NOx (mostly from lightning) into the upper troposphere


O3 production during transport and subsidence over South Atlantic basin

Sauvage et al., 2007


Conclusions

Global lightning NOx source likely between 4 – 8 Tg N / yr


6 Tg N / yr is a best estimate

Further refinement will require


- vertically-resolved constraint
- more observations (e.g. HNO3)
- improved satellite retrieval accuracy (e.g. NO2)
- stronger constraints on midlatitude source
- model development to better represent processes (e.g.
lightning NOx representation, vertical transport)

Acknowledgements
CFCAS and NASA

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