Deuterium enriched water vapor Fourier Transform Spectroscopy: the 8800-10800 cm -1 spectral region. (1) L. Daumont, (1) A. Jenouvrier, (2) S. Fally, (3)

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Presentation transcript:

Deuterium enriched water vapor Fourier Transform Spectroscopy: the cm -1 spectral region. (1) L. Daumont, (1) A. Jenouvrier, (2) S. Fally, (3) C. Hermans, (2) A. C. Vandaele and (2) M. Carleer (1)Université de Reims Champagne-Ardenne, Groupe de Spectrométrie Moléculaire et Atmosphérique, Reims, France. (2)Université Libre de Bruxelles, Service de Chimie Quantique et Photophysique, Brussels (ULB-SCQP), Belgium. (3)Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, Belgium.

Experimental setup The 50 meter base long multipass cell BRUKER IFS 120 M spectrometer Detector: Si Diode Quartz beamsplitter Stabilized W lamp Water vapor:

HOD D2OD2O HITRAN 2004 ICLAS + ICLAS- VeCSEL FTS Previous studies: Positions (and assignements)Intensities FTS+ ICLAS-VeCSEL FTSFTS+ ICLAS …cm -1 FTS Present Work

HITRAN 2004 Band Centers (cm -1 ) Band integrated absorption cross sections ΣS(296K) cm -1 /(molec/cm -2 ) HOD H 2 17 O H 2 18 O H 2 16 O 7513 cm -1

Raw spectra for different H 2 O/HDO/D 2 O mixtures Species identification P tot = P H2O + P HDO + P D2O - P H2O from BR list - P HDO and P D2O : (a)- Equilibrium constant ( Pred: Appl. Spectrosc. 49 (10) (1995) ) (b)- Mean ratios of the measured line areas in the spectra B and C. Better reproducibility of line intensities. Partial pressures Species HDOD 2 O Nbr of measured lines Nbr of assignments Nbr of unassigned lines Line parameters Assignments and partial pressures

4 22 KaKa Term values Example of Ritz energy difference: from the 3υ (cm -1 )

Example of HDO subband of ν 1 +2 ν 3 : S(obs) S(PS) ν obs -ν calc (cm -1 ) x S (cm molec -1 ) Average: 0.95

Contributions of the different species Integrated absorption cross sections cm -1 /(molec/cm -2 ) (293 K) Natural H 2 O D2OD2O HDO

D 2 O: the 3ν 1 +ν 3 band Positions obs = This work and Ulenikov* Absolute intensities Self-broadening coefficients Comparison between observed and calculated Mean ratio: 1.03 Wavenumbers (cm -1 ) ν obs -ν PS (cm -1 ) K max J max γ self (cm -1 /atm) Wavenumbers (cm -1 ) * Ulenikov JMS 210, 18 (2001)

D 2 O: the 2ν 1 +ν 2 +ν 3 band Positions Absolute intensities Self-broadening coefficients Comparison between observed and calculated Wavenumber cm -1 Mean ratio: 1.07 Wavenumber (cm -1 ) ν obs -ν PS (cm -1 ) K max J max γ self (cm -1 /atm)

Wavenumber (cm -1 ) ν obs -ν PS (cm -1 ) Comparison between observed and calculated positions D 2 O: the 2ν 1 +ν 2 +ν 3 band

Positions ν obs -ν PS (cm -1 ) J max K max Comparison between observed and calculated D 2 O: the 2ν 1 +ν 2 +ν 3 band

HDO: the 3ν 3 band. Positions Absolute intensities Self-broadening coefficients Comparison between observed and calculated Wavenumber cm -1 Mean ratio: ν obs -ν PS (cm -1 ) K max J max γ self (cm -1 /atm) J max K max

Summary: Line positions, assignements, intensities and self broadening parameters are now available for HDO and D 2 O in this region (soon on the web). The rovibrational assignement is close to be completed. Further work  Lower region: cm -1 (approximately lines of HDO and D 2 O to be measured).  H 2 18 O and H 2 17 O ? L. Daumont, A. Jenouvrier, S. Fally, C. Hermans, A. C. Vandaele and M. Carleer Deuterium enriched water vapor Fourier Transform Spectroscopy: the cm -1 spectral region. Part from the IUPAC task group on Water spectroscopic database built up (J. Tennyson) Financial support of the Programme National de Chimie Atmosphérique (France)

The cm -1 spectral region Natural H 2 O D 2 O-H 2 O mixture D 2 O + HDO H2OH2O