New 12 C 2 H 2 measurements using synchrotron SOLEIL David Jacquemart, Nelly Lacome, Olivier Piralli 66th OSU international symposium on molecular spectroscopy

New 12C2H2 measurements using

synchrotron SOLEIL

David Jacquemart, Nelly Lacome, Olivier Piralli

66th OSU international symposium on molecular spectroscopy 2011 – WF08

FTS (Bruker 125HR) and synchrotron source around 100 µm (100 cm-1)

→ HERSHEL space observatory – instrument PACS (up to 160 cm-1)

In Saint-Aubin located at a few kilometers from Paris

→ Use of synchrotron source SOLEIL (AILES beamline)


http://images.google.com/imgres?imgurl=https://www.imagif.cnrs.fr/uploads/partners/medium/1205277524_1203405092_logo%2520soleil.jpg&imgrefurl=https://www.imagif.cnrs.fr/partners_details.php%3Fid_partner%3D28&usg=__oYBwk1P51-lYT8fJWisz9XWEL1I=&h=140&w=210&sz=14&hl=fr&start=3&um=1&tbnid=gOsi-RhV9T1OeM:&tbnh=71&tbnw=106&prev=/images%3Fq%3Dsoleil%2Bsynchrotron%26hl%3Dfr%26rls%3Dcom.microsoft:fr:IE-SearchBox%26rlz%3D1I7GGLR%26sa%3DN%26um%3D1


Experimental conditions for 2010 SOLEIL spectra

→ Use of a multispectrum fitting procedure to retrieve line positions and intensities with a Voigt profile


2009

2010

Water transitions

Acetylene from Kabbadj et al.


In 2010, using 150 m absorption path: P(C2H2)= 0.25, 0.6, 2, and 5 mbar


Michelson-type Interferometer

)]([)2cos()()(2)(0

1 BTFdBI

Limitation of the optical path difference

)().()( 0 maxII

( ) 1 for 0 ,

( ) 0 for .max

max

max

max

maxexp 0( ) ( ) ( ). ( ) ( ) ( )

max thT TF I TF I B f

Recent progress in acetylene laboratory measurements for astrophysical applications, EGU General Assembly 3-8 April 2011

( ) ( ) 2 sin (2 )max max max maxf TF c

Effects of the size of the beam

2sin)( 0 cPopt

2

2

fR

)().().()( 0 optPIImax

)().()( optPTFfmax

I’ () sin (0 / 2) / (0 / 2) cos [2 0 (1 /4)]

Shift of the positions to lower wavenumbers of a quantity equal to 0/4

Optical weighting of the rectangular function (boxcar)

Apodization of the sinc


Classical source (globar…)Classical source (globar…)

Radius of the beam delimited by an iris.

The size of the beam in the interferometer is a constant physical parameter.

Synchrotron source (AILES)Synchrotron source (AILES)

Radius of the beam not delimited by an iris.The size of the beam in the interferometer is depending on the photons energies. (SOLEMIO and SRW models) At 10 cm-1, diameter of 7 mm At 100 cm-1, diameter of 2.5 mm At 1000 cm-1, diameter of 0.8 mm

2sin)( 0 cPopt 2

2

fR

0 500 1000 1500 20000.0

0.2

0.4

0.6

0.8

1.0

max

= 450 cm

(res bruker = 0.002 cm-1)

R = 3.00 mm; f = 418 mm

Op

tical

we

ight

ing

Optical path difference in cm

300 cm-1

100 cm-1

50 cm-1

10 cm-1

The size of the beam is known (even if slight differences from diffraction effects).The optical weighting is wavenumber dependent !

0 500 1000 1500 20000.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1.0

1.1

max

= 900 cm

res bruker = 0.001 cm-1

Op

tica

l we

igh

ting

Optical path difference in cm

10 cm-1; R=3.5 mm

100 cm-1; R=1.25 mm

1000 cm-1; R=0.4 mm

2

20 max

2R

f


The size of the beam is not constant according to wavenumbers.The optical weighting is almost constant according to wavenumbers.


2009 SOLEIL spectra

Effective iris radius from line by fine fitting

(H216O in open symbols and 12C2H2 in

solid ones)


-100 0 100 200 300 400 500 600 700 800 900 1000 11000.0

0.5

1.0

1.5

2.0

2.5

3.0

3.5

4.0

Wavenumbers in cm-1

Spectrum #1

Eff

ect

ive

ra

diu

s o

f th

e b

ea

m in

mm

2010 SOLEIL spectra


(H216O in red symbols and 12C2H2 in

black ones)


2010 SOLEIL spectra



black ones)

-100 0 100 200 300 400 500 600 700 800 900 1000 11000.0

0.5

1.0

1.5

2.0

2.5

3.0

3.5

4.0

Eff

ect

ive

ra

diu

s o

f th

e b

ea

m in

mm

Wavenumbers in cm-1

Spectrum #2


2010 SOLEIL spectra



black ones)

-100 0 100 200 300 400 500 600 700 800 900 1000 11000.0

0.5

1.0

1.5

2.0

2.5

3.0

3.5

4.0E

ffe

ctiv

e r

ad

ius

of

the

be

am

in m

m Spectrum #3

Wavenumbers in cm-1


2010 SOLEIL spectra



black ones)

-100 0 100 200 300 400 500 600 700 800 900 1000 11000.0

0.5

1.0

1.5

2.0

2.5

3.0

3.5

4.0

Wavenumbers in cm-1

Eff

ect

ive

ra

dius

of t

he b

eam

in m

m

Spectrum #4


2010 SOLEIL spectra



black ones)

0 100 200 300 400 500 600 700-0.5

0.0

0.5

1.0

1.5

2.0

2.5

3.0

3.5

4.0

Eff

ect

ive

iris

ra

diu

s in

mm

Wavenumbers in cm-1

Spectrum #0 recorded using iris radius = 0.9 mm


0 100 200 300 400 500

-1.0x10-6

0.0

1.0x10-6

2.0x10-6

3.0x10-6

4.0x10-6

Wavenumber in cm-1

(H

ITR

AN- ob

s) / H

ITR

AN

Wavenumber calibration using H2O transitions(open circles in spectrum #0, open squares in #1, solid squares in # 2, solid triangles in # 3 and open triangles in #4)

and NH3 transitions (open stars in spectrum #1)

50 100 150 200 2504.0x10-5

6.0x10-5

8.0x10-5

1.0x10-4

1.2x10-4

1.4x10-4

1.6x10-4

1.8x10-4

2.0x10-4

2.2x10-4

obs- H

ITR

AN

Wavenumbers in cm-1


Transition dipole moment for the 51 - 4

1 band

-30 -20 -10 0 10 20 30 40 50

5.0x10-4

1.0x10-3

1.5x10-3

2.0x10-3

2.5x10-3

3.0x10-3

Tra

nsiti

on d

iopo

le m

omen

t squ

ared

(in

Deb

ye2 )

m

Pee

and Ree

sub branches P

ff and R

ff sub branches

Qfe sub branch

Qef sub branch

[Jac10] [Amy10]

[Amy10] Amyay B., Herman M., Fayt A., Fusina L, Predoi-Cross A.. Chemical Physics Letters 491:17 (2010).

[JAC10] Jacquemart D., Gomez L., Lacome N., Mandin J.-Y., Pirali O., Roy P. JQSRT 111, 1223-1233 (2010).


-30 -20 -10 0 10 20 30 402.0x10-3

3.0x10-3

4.0x10-3

5.0x10-3

6.0x10-3

7.0x10-3

8.0x10-3

9.0x10-3

1.0x10-2

1.1x10-2

1.2x10-2

1.3x10-2

1.4x10-2

1.5x10-2 P

ee and R

ee sub branches

Pff and R

ff sub branches

Qfe sub branch

Qef sub branch

[Amy10]Qef sub branch

Qfe sub branch

m

Tra

nsiti

on d

iopo

le m

omen

t squ

ared

(in

Deb

ye2 )

Transition dipole moment for the (4+ 5)2 - 242

band


-30 -20 -10 0 10 20 30 40 50

0.0

1.0x10-3

2.0x10-3

3.0x10-3

4.0x10-3

5.0x10-3

m

Tra

nsiti

on d

iopo

le m

omen

t squ

ared

(in

Deb

ye2 )

Transition dipole moment for the (4+ 5)0 - 242

band

(forbidden band with ∆ℓ=2)


-40 -30 -20 -10 0 10 20 30 40 504.0x10-3

4.2x10-3

4.4x10-3

4.6x10-3

4.8x10-3

5.0x10-3

5.2x10-3

5.4x10-3

5.6x10-3

5.8x10-3

Tra

nsiti

on d

iopo

le m

omen

t squ

ared

(in

Deb

ye2 )

m

Transition dipole moment for the 250

- (4+ 5)0+ band

Conclusion

- Better signal to noise ratio in 2010 than in 2009

(mainly due to the bolometer)

- Smaller dispersion of the radius of the beam

(more accurate model of apparatus function)

- Absolute line positions and intensities retrievals (for 816 transitions belonging to 17 bands between 51 and 215 cm-

1)


Thank you for your attention


Kabbadj Y, Herman M, Di Lonardo G, Fusina L, Johns JWC. JMS 150:535 (1991)

D. Jacquemart, L. Gomez, N. Lacome, J.-Y. Mandin, O. Pirali, P. Roy, JQSRT 110: 2102 (2009)

SOLEIL-AILESSOLEIL-AILES ((2009)2009)White cell with 10m absorption path, pressure of acetylene between 0.5 – 10 mbar (50-600 cm-1) 10 bands observed, Line intensities retrievals for the strongest ν5 – ν4 band

B. Amyay, M. Herman, A. Fayt, L. Fusina, A. Predoi-Cross. Chemical Physics Letters 491:17 (2010)

Canadian Light Source, Saskatoon 2009-2010Canadian Light Source, Saskatoon 2009-2010

White cell with 72m absorption path, pressure of acetylene between 1 – 4 mbar (46-246cm-1) 20 bands observed positions and intensities calculation (constant vibrational dipole moment)

D. Jacquemart, N. Lacome, O. Pirrali. (to be submitted)

SOLEIL-AILES (SOLEIL-AILES (2010)2010)

White cell with 150m absorption path, pressure of acetylene between 0.1 – 10 mbar (50-600 cm-1) 10 +38 bands observed, Line intensities retrievals for at least 15 weak bands (to be submitted)

One FT spectrum res = 0.001-4 cm-1

White cell with 18m absorption path100-400 Pa10 bands observed, Line positions analysis

Documents

New 12 C 2 H 2 measurements using synchrotron SOLEIL David Jacquemart, Nelly Lacome, Olivier Piralli 66th OSU international symposium on molecular spectroscopy