Determining emissions of environmentally important

gases using data from aircraft and satellites

with Dorian Abbot, Arlene Fiore, Colette Heald, Daniel Jacob, Dylan Jones, Jennifer Logan, Loretta Mickley, Bob Yantosca

Harvard UniversityRandall Martin, Kelly Chance, Thomas Kurosu

Harvard-SmithsonianGlen Sachse NASA Langley; Don Blake UCI;David Streets Argonne National Laboratory;

Henry Fuelberg, Chris Kiley FSU

http://www.people.fas.harvard.edu/~ppalmer

Paul Palmer

Global 3d chemistry transport

model

Top-down and bottom-up emission inventories

GOME,

MOPITT,

SCIAMACHY

TES, OMI

CMDL network for CO and CO2

CO inverse modeling•Product of incomplete combustion; main sink is OH

•Lifetime ~1-3 months

•Relative abundance of observations

•Previous studies found a discrepancy between Asian emission inventories and observations

RH + OH … CO

1000s km

Direct & indirect emissions

CMDL site

Many 100s km10s km

Increasing model transport error

Limitation of remote data for inverse model calculations

TRACE-P data can improve level of disaggregation of continental emissions

110 E 120 E 130 E 140 E 150 E 160 E

Longitude

0 N

10 N

20 N

30 N

40 N

50 N

Lat

itu

de

DC-8 FlightsP-3B Flights

cold front

cold air

warm air

Main transport processes:

DEEP CONVECTION

OROGRAPHIC LIFTING

FRONTAL LIFTING

100 E 130 E 160 E 190 E 220 E 250 E 280 E

Longitude

0 N

10 N

20 N

30 N

40 N

50 N

60 N

La

titu

de

DC-8 FlightsP-3B Flights

Feb – April 2001

Forward model (GEOS-CHEM)

Inverse model

P3B, DC8 observations y

Emissions x

FF

BB

BF

Modeling Overview

xs = xa + (KTSy-1K + Sa

-1)-1 KTSy-1(y – Kxa)

SS = (KTSy-1K + Sa

-1)-1

y = Kxa +

DACOM (Sachse)

TRACE-P CO Emissions Inventories Biomass

burning: Variability from observed daily firecount data (AVHRR)

(Heald/Logan)

Anthropogenic emissions for Y2K1 (fuel consumption)

(Streets)

Tagged model CO simulation for TRACE-P

ChinaJapan

Southeast Asia

Korea

Rest of World

[OH] from full-chemistry model (CH3CCl3 = 6.3 years)

Global 3D CTM 2x2.5 deg resolution

GEOS-CHEM

CO

[p

pb

]

Lat [deg]

Observation

A priori

A priori emissions have a large negative bias in the boundary layer

xs = xa + (KTSy-1K + Sa

-1)-1 KTSy-1(y – Kxa)

SS = (KTSy-1K + Sa

-1)-1

x = state vector (emissions)y = observation vector (TRACE-P CO, ppb)

Choice of state vector…-Aggregate anthropogenic emissions-Aggregate Korea/Japan

Inverse Model (a.k.a. Weighted linear least-

squares)

Gain matrix

o Emission uncertainties for Asia Sa :

Anthropogenic (D. Streets): China (78%), Japan (17%), Southeast Asia (100%), Korea (42%)

Biomass burning: 50%; Chemistry (largely CH4): 25%

o Observation uncertainty Sy :

Measurement accuracy (1%)

Representation (14ppb or 25%):

Model errors…

GEOS-CHEM

GEOS-CHEM

2x2.5 cell

TRACE-P

Error specification is crucial

Estimated: 1 sigma value about mean observed 2x2.5 value

All latitudes

(measured-model) /measured

Alt

itu

de [

km

]

Mean bias

RRE

Model error: (y*RRE)2 ~38ppb (>70% of total

observation error)

MODEL ERROR

Kore

a +

Jap

an

Sou

theast

Asia

Ch

ina (

BB

)

Ch

ina

(an

thro

pog

en

ic)

A prioriA posteriori

1-sigma uncertaint

y

Rest of World

Our best estimate is insensitive to inverse model assumptions

GEOS-CHEM

CO

[p

pb

]

Lat [deg]

Observation

A priori

A posteriori

A posteriori emissions improve agreement with observations

[1018 molec cm-2]

MOPITT shows low CO columns over Southeast Asia during TRACE-P

GEOS-CHEM

MOPITT

MOPITT – GEOS-CHEM

[1018 molec cm-2]c/o Heald, Emmons, Gille

Largest difference

Next steps with CO…

Multi-species inversion will bring additional information:

-CH3CN will bring information about biomass burning

-CO2 used to disaggregate emissions from Korea and Japan (CO2/CO)

Direct & indirect emissions

Can calculate emissions of anthropogenic halocarbon X given the X:CO slope and CO emissions

Western Pacific

CO, species with CO, +many other species

Asian continent

Blake group: CH3CCl3, CCl4, Halons 1211, 1301, 2402, CFCs 11, 12, 113, 114, 115

2 kmFresh

emissions

Back-trajectories of top 5% of observed values indicate local

sources

Proxy for OHOnly a strong local source

CO:CH3CCl3 relationships

= value above

“background”

0

5

10

15

20

25

30

35

40

45

Gg

/yr

CH 3CCl 3

CCl 4

CFC-11

CFC-12

CH3CCl3,CCl4,CFCs 11 & 12):

-represents >80% of East Asia ODP (70% of total global ODP)

-103.1 ODP Gg/yr (East Asia)

East Asia ODP = 70%

Global ODP = 20%

Eastern Asia estimates

Large global & regional implications

Methodology has the potential to monitor magnitude and trends of emissions of a wide range of environmentally important gases

Previous workThis work

0.9

1.4

2.3

3.0

Platform multiple ERS-2 Terra ENVISAT Space station

Aura TBD TBD

Sensor TOMS GOME MOPITT MODIS/MISR

SCIAMACHY MIPAS SAGE-3 TES OMI MLS CALIPSO OCO

Launch 1979 1995 1999 1999 2002 2002 2004 2004 2004 2004 2004 2005

O3 N N/L L L N/L N L

CO N N/L L N/L

CO2 N/L N

NO L

NO2 N N/L N

HNO3 L L

CH4 N/L N

HCHO N N/L N

SO2 N N/L N

BrO N N/L N

HCN L

aerosol N N N L N N

N = NadirL = Limb

Satellite data will become integral to the study of tropospheric chemistry in the next

decade

• Nadir-viewing SBUV instrument

• Pixel 320 x 40 km2

• 10.30 am cross-equator time

• Global coverage in 3 days

Global Ozone Monitoring Experiment

•HCHO slant columns fitted: 337-356nm

- fitting uncertainty 4 x 1015 molec cm-2HCHO JULY 1997

Isoprene

Biomass Burning

Isoprene dominates HCHO production over US during

summer Southern Oxidant Study 1995

North Atlantic Regional Experiment 1997

[ppb]

Surface source (mostly isoprene+OH)

Continental outflow

Alt

itu

de

[km

]

Alt

itu

de

[km

]

measurements GEOS-CHEM model

Defined background CH4 + OH

Using HCHO Columns to Map Isoprene Emissions

isoprene

HCHOhours

OH

hours

Displacement/smearing length scale 10-100 km

h, OH

EISOP = ___________kHCHO HCHO

Yield ISOPHCHO

[1016molec cm-2]

GEOS-CHEM GOME

r2 = 0.7 n = 756Bias = 11%

HCHO columns – July 1996HCHO columns – July 1996

Model:Observed HCHO columns

GEIA isoprene emissions

[1012 atoms C cm-2 s-

1]

BIOGENIC ISOPRENE IS THE MAIN SOURCE OF HCHO IN U.S. IN SUMMER

[1012 atom C cm-2 s-

1]

GOME isoprene emissions (July 1996) agree with surface measurements

r2 = 0.77

Bias -12%

50

GEOS-CHEMGOME GOME GEOS-CHEM

1016 molecules cm-2

SEASONAL VARIABILITY IN GOME HCHO COLUMNS

0 2.5

r>0.75bias~20%

MAR

APR AUG

MAY

JUN

SEP

JUL

OCT

•Interannual Variability ~30%

10

16 m

ole

cu

les c

m-2

°C

0

2.5

-2

2

GOME T GOME

95

INTERANNUAL VARIABILITY IN GOME HCHO COLUMNS (1995-2001)

August Monthly Means & Temperature AnomalyT

97

98

01

00

99

96