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First global observation of organic compounds
from the IASI infrared sounder:
HCOOH and CH3OH
Federico Karagulian1, Lieven Clarisse1,
Ariane Razavi1, Cathy Clerbaux2, Pierre Coheur1,
Daniel Hurtmans1 ,Trissevgeni Stavrakou3 and
Jean-François Müller3
1Spectroscopie

de l’Atmosphere, Sevice de Chimie Quantique et de Photophysique,
Université Libre de Bruxelles, Brussels, Belgium
2UPMC Univ. Paris 06; Université Versailles St-Quentin; CNRS/INSU, LATMOS-IPSL, Paris, France.
3Belgian Institute for Space Aeronomy, Brussels, Belgium
IASI

IASI instrument and observing mode
(Infrared Atmospheric Sounding Interferometer)
MetOp: First European meteorological platform on
polar orbit (EPS system)

MetOP
IASI
Nadir looking FTS

• 12 km pixel x 4 @ nadir
• 120 spectra along the swath (±48.3° Scan
2400 km), each 50 km along the trace

Small ground pixel size
Global coverage twice
daily (morning and
evening orbits)

IASI

• Spectral coverage = 645-2760 cm-1
• Spectral resolution = 0.5 cm-1
• Radiometric noise ~ <0.1-0.2 K

Broad spectral
coverage without
gaps
Medium spectral resolution
High radiometric performances
IASI

IASI instrument and observing mode
Level 1 radiance spectrum

1.4x10

-5

1.2x10
1.0x10

-5

8.0x10

-6

4.0x10

-6

2

2

-6

6.0x10

CO

Radiance accuracy
within 0.5 K above
ocean

-5

-1

Radiance (W / cm sr cm )

SA/CNRS – ULB ULB
LATMOS/IPSL HNO3
CFC11, CFC12

2.0x10

O3

Illingworth et al., ACPD 2009

CH3OH

CO

HCOOH
CO2, N2O

Ts=275 K

N2O, CH4
16
H2 O, HOD

HOD

16
H2 O
-6

Thermal +
reflected solar
radiation
(daytime)

CH4

18
H2 O

0.0
800 1000 1200 1400 1600 1800 2000 2200 2400 2600
-1

Wavenumber (cm )
Trace gases

IASI contribution to atmospheric composition measurements
IASI species

10 Years

Year

Day

HCOOH
CH3OH

Hemispheric mixing:
~1-2 months
PBL mixing:
~few hours

CO
O3
HNO3
SO2
H2O + Iso
VOCs

NH3

hour.

HCOOH
CH3OH

Chemistry and sources

Month

Global mixing
~1 year

CFC11
N2O
CO2
CH4
OCS

Chemistry and transport

CO2

climate

CFC12

Sec.

IASI ACP special issue
With about 25 papers
HCOOH
CH3OH

Influence on the global
radiative forcing
SOURCES OF FORMIC ACID (HCOOH)
Use the IMAGESv2 global CTM* to simulate HCOOH
HCOOH lifetime: 7 days
Global annual HCOOH emission: 8.9 Tg/yr

Biogenic Emissions
MEGAN-ECMWF
(Muller et al. 2008)

Secondary

EDGARv3.3
Primary + secondary

Biogenic
72%
ISOPRENE
Terpenes
Ethene (C2H4)

Anthrop.
12%

Biomass
burning
16%

Primary + secondary
Ethyne C2H2
Hydroxacetone
Glycolaldehyde

Pyorogenic emissions
GFEDv2
(Van der Werf et al. 2006)

*Belgian Institute for Space Aeronomy (IASB-BIRA)
SOURCES OF methanol (CH3OH)
Use of IMAGESv2* to simulate CH3OH
CH3OH lifetime: 9 days
Global annual CH3OH emission: 204 Tg/yr

Biogenic Emissions

Biogenic Emissions
Primary

Plant
growth
65%

Plant
decay 11%

Primary

CH4 oxid. 12 %
VOCs oxid. 4%
Anthropogenic 5%
Fires 3%
*Belgian Institute for Space Aeronomy
(IASB-BIRA)
HCOOH observation in USA: retrieval with Atmosphit
1.00

(baseline); 1105
(target)
for the calculation of the Brightness
Temperature Difference (BTD)
cm-1

0.98
Trasmittance (a.u)

1103-1109cm-1

0.96
0.94
0.92
0.90
0.88
0.86

IASI Radiance spectrum

HCOOH
(reference)

1070

1080

Brightness Temperature (K)

HCOOH

2

-1

Radiance (W/m sr m )

1.0
0.8
0.7

H2O

0.6
0.5
0.4

2

-1

RMS = 2.746e-06 (W/m sr m )
2
[HCOOH] = 1.31e+16 molec/cm )

1103

1104

1105 1106 1107
-1
wavenumber (cm )

1108

1109

Averaging Kernels for total HCOOH column

-1

1090 1100 1110 1120
-1
wavenumber (cm )

-3

1.1x10

0.9

1105 cm

0.84
1130

1140

320
315
310
305
300

HCOOH x 10

295
290
285
1103

IASI spectrum in BT
Simulation of HCOOH
1104

H2O

1105
1106
1107
-1
wavenumber (cm )

1108

1109

Profiles

DOFland = 1.25
DOFocean = 1.5

Used a priori profile from IMAGESv2 model
Retrievals for HCOOH in the region (1103.74-1109.75 cm-1): USA

(1016 molec./cm2)

(Kelvin)

Countries

Slope(*)

Australia

0.8339

China

0.7049

USA

0.6187

East EU

0.7409

India

0.7301

Brazil

0.7719

Africa

0.7126

Mexico

0.6643

-2

HCOOH column (10 molec./cm )

 0-18 km  6 partial columns of 3 km thickness
 Good correlation between HCOOH column and BTD

2.0

Correlation = 0.892

16

1.5
1.0
0.5
-2

slope = 0.618e+16 (molec./cm )/K
R=0.8922

0.0
0.0

0.5

1.0

1.5
2.0
BTD (K)

2.5

3.0

3.5

(*)HCOOH

total column (1016 molec./cm2)/ BTD (K)
IMAGESv2 model 2008 (HCOOH: January 2008 - December 2008)
anthropogenic

biomass burning
biogenic

biomass burning

biogenic

A priori [HCOOH] total column = 2.9074e+15 molec./cm2
HCOOH Total Column (June 2008 - May 2009)
biogenic not seen
anthrop. in the model

anthrop. biogenic

biomass burning
HCOOH column (1014 molec./cm2)

biogenic
biomass burning
anthtop.

biomass burning
biogenic

anthrop.

biogenic
biomass burning
HCOOH Total Column (June 2008 - May 2009)
First background filtering: transport observed

biogenic not seen
anthrop. in the model

anthrop.

biogenic

anthrop.
biomass burning
biogenic

biogenic
biomass burning

no HCOOH observed above tropical forests

HCOOH column (1014 molec./cm2)

biogenic
biomass burning
anthtop.

biomass burning
Difference between IASI (filtered) and BIRA model (2008)

HCOOH column (1014 molec./cm2)

Mainly biogenic HCOOH emissions
over tropical forests
Correlation between HCOOH and CO emissions from fires in Africa

(1018 molec./cm2)

HCOOH column (10

16

2

molec./cm )

(1016 molec./cm2)

3.0

Savanna burning

Correlation factor = 0.9

Fires
(from MODIS)

2.5
2.0
1.5

CO emission

1.0
0.5

1.5

2.0
2.5
3.0
3.5
18
2
CO column (10 molec./cm )

HCOOH/CH3OH
emission

4.0

High correlation
Correlation between HCOOH and CH3OH; biogenic emissions?

(HCOOH) BTD (K)

(1018 molec./cm2)

(Kelvin)

(1016 molec./cm2)

1.6

Fires

 Good correlation between
HCOOH and CH3OH

correlation factor = 0.702

 Low correlation between CO
emission from fire and HCOOH/CH3OH

1.2
0.8
0.4

Not only biomass
burning

0.0
0.0

0.5

1.0
(CH3OH) BTD (K)

1.5

2.0

HCOOH and CH3OH might be correlated to
biogenic emissions (in addition to biomass burning)
CH3OH (September 2008 - July 2009)
anthropogenic

IASI Radiance spectrum (Mexico)
-5

1.0x10

20090508

-6

-1

radiance [W/m sr m ]

5.0x10

2

0.0

-6

-5.0x10

residue
residue - ch3oh
ch3oh simulated

-5

-1.0x10

-5

-1.5x10

-5

-2.0x10

1030

rms=2.650e-6
1040

1050

BT=1.072
1060

1070

1080

-1

wavenumber [cm ]

biomass burning
biogenic

Mainly plant growth
emissions from the
model IMAGESv2

CH4 oxidation
Correlation between vegetation and HCOOH emissions

cultivated
shrubs

desert

shrubs

shrubs

desert

herbaceous
shrubs

cultivated

trees
trees
shrubs
shrubs
cultivated
herbaceous
grass

shrubs

Not only biomass
burning

http://www.fao.or/
Correlation between vegetation in Africa and HCOOH
Biomass
burning
+
biogenic
desert
April 09

herbaceous
March 09
shrubs
trees
August 08

shrubs

shrubs
October 08
grass
Conclusions

 First global observations of HCOOH and CH3OH
(still at a qualitative level)

Sources
Transport

 Preliminary comparison with model IMAGESv2 shows
some correlations.
 Additional observation from IASI show:
 Not seen biogenic emissions above tropical forests
 Biogenic emissions above shrublands
 Anthropogenic emissions over the US and India

Outlook
 Optimization of the background filtering
 Optimization in the assignation of anthropogenic
and HCOOH/CH3OH biogenic emissions

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Satellite Remote Sensing (Formic Acid)

  • 1. First global observation of organic compounds from the IASI infrared sounder: HCOOH and CH3OH Federico Karagulian1, Lieven Clarisse1, Ariane Razavi1, Cathy Clerbaux2, Pierre Coheur1, Daniel Hurtmans1 ,Trissevgeni Stavrakou3 and Jean-François Müller3 1Spectroscopie de l’Atmosphere, Sevice de Chimie Quantique et de Photophysique, Université Libre de Bruxelles, Brussels, Belgium 2UPMC Univ. Paris 06; Université Versailles St-Quentin; CNRS/INSU, LATMOS-IPSL, Paris, France. 3Belgian Institute for Space Aeronomy, Brussels, Belgium
  • 2. IASI IASI instrument and observing mode (Infrared Atmospheric Sounding Interferometer) MetOp: First European meteorological platform on polar orbit (EPS system) MetOP IASI Nadir looking FTS • 12 km pixel x 4 @ nadir • 120 spectra along the swath (±48.3° Scan 2400 km), each 50 km along the trace Small ground pixel size Global coverage twice daily (morning and evening orbits) IASI • Spectral coverage = 645-2760 cm-1 • Spectral resolution = 0.5 cm-1 • Radiometric noise ~ <0.1-0.2 K Broad spectral coverage without gaps Medium spectral resolution High radiometric performances
  • 3. IASI IASI instrument and observing mode Level 1 radiance spectrum 1.4x10 -5 1.2x10 1.0x10 -5 8.0x10 -6 4.0x10 -6 2 2 -6 6.0x10 CO Radiance accuracy within 0.5 K above ocean -5 -1 Radiance (W / cm sr cm ) SA/CNRS – ULB ULB LATMOS/IPSL HNO3 CFC11, CFC12 2.0x10 O3 Illingworth et al., ACPD 2009 CH3OH CO HCOOH CO2, N2O Ts=275 K N2O, CH4 16 H2 O, HOD HOD 16 H2 O -6 Thermal + reflected solar radiation (daytime) CH4 18 H2 O 0.0 800 1000 1200 1400 1600 1800 2000 2200 2400 2600 -1 Wavenumber (cm )
  • 4. Trace gases IASI contribution to atmospheric composition measurements IASI species 10 Years Year Day HCOOH CH3OH Hemispheric mixing: ~1-2 months PBL mixing: ~few hours CO O3 HNO3 SO2 H2O + Iso VOCs NH3 hour. HCOOH CH3OH Chemistry and sources Month Global mixing ~1 year CFC11 N2O CO2 CH4 OCS Chemistry and transport CO2 climate CFC12 Sec. IASI ACP special issue With about 25 papers HCOOH CH3OH Influence on the global radiative forcing
  • 5. SOURCES OF FORMIC ACID (HCOOH) Use the IMAGESv2 global CTM* to simulate HCOOH HCOOH lifetime: 7 days Global annual HCOOH emission: 8.9 Tg/yr Biogenic Emissions MEGAN-ECMWF (Muller et al. 2008) Secondary EDGARv3.3 Primary + secondary Biogenic 72% ISOPRENE Terpenes Ethene (C2H4) Anthrop. 12% Biomass burning 16% Primary + secondary Ethyne C2H2 Hydroxacetone Glycolaldehyde Pyorogenic emissions GFEDv2 (Van der Werf et al. 2006) *Belgian Institute for Space Aeronomy (IASB-BIRA)
  • 6. SOURCES OF methanol (CH3OH) Use of IMAGESv2* to simulate CH3OH CH3OH lifetime: 9 days Global annual CH3OH emission: 204 Tg/yr Biogenic Emissions Biogenic Emissions Primary Plant growth 65% Plant decay 11% Primary CH4 oxid. 12 % VOCs oxid. 4% Anthropogenic 5% Fires 3% *Belgian Institute for Space Aeronomy (IASB-BIRA)
  • 7. HCOOH observation in USA: retrieval with Atmosphit 1.00 (baseline); 1105 (target) for the calculation of the Brightness Temperature Difference (BTD) cm-1 0.98 Trasmittance (a.u) 1103-1109cm-1 0.96 0.94 0.92 0.90 0.88 0.86 IASI Radiance spectrum HCOOH (reference) 1070 1080 Brightness Temperature (K) HCOOH 2 -1 Radiance (W/m sr m ) 1.0 0.8 0.7 H2O 0.6 0.5 0.4 2 -1 RMS = 2.746e-06 (W/m sr m ) 2 [HCOOH] = 1.31e+16 molec/cm ) 1103 1104 1105 1106 1107 -1 wavenumber (cm ) 1108 1109 Averaging Kernels for total HCOOH column -1 1090 1100 1110 1120 -1 wavenumber (cm ) -3 1.1x10 0.9 1105 cm 0.84 1130 1140 320 315 310 305 300 HCOOH x 10 295 290 285 1103 IASI spectrum in BT Simulation of HCOOH 1104 H2O 1105 1106 1107 -1 wavenumber (cm ) 1108 1109 Profiles DOFland = 1.25 DOFocean = 1.5 Used a priori profile from IMAGESv2 model
  • 8. Retrievals for HCOOH in the region (1103.74-1109.75 cm-1): USA (1016 molec./cm2) (Kelvin) Countries Slope(*) Australia 0.8339 China 0.7049 USA 0.6187 East EU 0.7409 India 0.7301 Brazil 0.7719 Africa 0.7126 Mexico 0.6643 -2 HCOOH column (10 molec./cm )  0-18 km  6 partial columns of 3 km thickness  Good correlation between HCOOH column and BTD 2.0 Correlation = 0.892 16 1.5 1.0 0.5 -2 slope = 0.618e+16 (molec./cm )/K R=0.8922 0.0 0.0 0.5 1.0 1.5 2.0 BTD (K) 2.5 3.0 3.5 (*)HCOOH total column (1016 molec./cm2)/ BTD (K)
  • 9. IMAGESv2 model 2008 (HCOOH: January 2008 - December 2008) anthropogenic biomass burning biogenic biomass burning biogenic A priori [HCOOH] total column = 2.9074e+15 molec./cm2
  • 10. HCOOH Total Column (June 2008 - May 2009) biogenic not seen anthrop. in the model anthrop. biogenic biomass burning HCOOH column (1014 molec./cm2) biogenic biomass burning anthtop. biomass burning biogenic anthrop. biogenic biomass burning
  • 11. HCOOH Total Column (June 2008 - May 2009) First background filtering: transport observed biogenic not seen anthrop. in the model anthrop. biogenic anthrop. biomass burning biogenic biogenic biomass burning no HCOOH observed above tropical forests HCOOH column (1014 molec./cm2) biogenic biomass burning anthtop. biomass burning
  • 12. Difference between IASI (filtered) and BIRA model (2008) HCOOH column (1014 molec./cm2) Mainly biogenic HCOOH emissions over tropical forests
  • 13. Correlation between HCOOH and CO emissions from fires in Africa (1018 molec./cm2) HCOOH column (10 16 2 molec./cm ) (1016 molec./cm2) 3.0 Savanna burning Correlation factor = 0.9 Fires (from MODIS) 2.5 2.0 1.5 CO emission 1.0 0.5 1.5 2.0 2.5 3.0 3.5 18 2 CO column (10 molec./cm ) HCOOH/CH3OH emission 4.0 High correlation
  • 14. Correlation between HCOOH and CH3OH; biogenic emissions? (HCOOH) BTD (K) (1018 molec./cm2) (Kelvin) (1016 molec./cm2) 1.6 Fires  Good correlation between HCOOH and CH3OH correlation factor = 0.702  Low correlation between CO emission from fire and HCOOH/CH3OH 1.2 0.8 0.4 Not only biomass burning 0.0 0.0 0.5 1.0 (CH3OH) BTD (K) 1.5 2.0 HCOOH and CH3OH might be correlated to biogenic emissions (in addition to biomass burning)
  • 15. CH3OH (September 2008 - July 2009) anthropogenic IASI Radiance spectrum (Mexico) -5 1.0x10 20090508 -6 -1 radiance [W/m sr m ] 5.0x10 2 0.0 -6 -5.0x10 residue residue - ch3oh ch3oh simulated -5 -1.0x10 -5 -1.5x10 -5 -2.0x10 1030 rms=2.650e-6 1040 1050 BT=1.072 1060 1070 1080 -1 wavenumber [cm ] biomass burning biogenic Mainly plant growth emissions from the model IMAGESv2 CH4 oxidation
  • 16. Correlation between vegetation and HCOOH emissions cultivated shrubs desert shrubs shrubs desert herbaceous shrubs cultivated trees trees shrubs shrubs cultivated herbaceous grass shrubs Not only biomass burning http://www.fao.or/
  • 17. Correlation between vegetation in Africa and HCOOH Biomass burning + biogenic desert April 09 herbaceous March 09 shrubs trees August 08 shrubs shrubs October 08 grass
  • 18. Conclusions  First global observations of HCOOH and CH3OH (still at a qualitative level) Sources Transport  Preliminary comparison with model IMAGESv2 shows some correlations.  Additional observation from IASI show:  Not seen biogenic emissions above tropical forests  Biogenic emissions above shrublands  Anthropogenic emissions over the US and India Outlook  Optimization of the background filtering  Optimization in the assignation of anthropogenic and HCOOH/CH3OH biogenic emissions