New analysis of the 3 & 4 bands of HNO 3 by high resolution Fourier transform spectroscopy in the 7.6 µm region

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1 New analysis of the 3 & 4 bands of HNO 3 by high resolution Fourier transform spectroscopy in the 7.6 µm region Agnés Perrin,, J.M.Flaud Laboratoire Interuniversitaire des Systémes Atmosphériques (LISA), CNRS, Université Paris Est, Créteil M.Ridolfi, M.Carlotti, Dipartimento di Chimica Fisica e Inorganica (DCFI), Universiy of Bologna, Viale del Risorgimento, , - Bologna, Italy. Agnes.Perrin@lisa.u-pec.fr A.Perrin: ASA-HITRAN 2012

2 HNO 3 in HITRAN-GEISA Intensities MW & 9 { 5,2 9 ) { 4, 3 } cm cm , 896cm , 1326cm cm -1 Far-IR 22µm 11µm 7.6µm 5.8µm Spectral range covered by ACE-FTS & MIPAS A.PerrinASA-HITRAN 2012

3 Intensities Up to now HNO 3 is measured (almost only) in the 11 µm region Which was updated recently in HITRAN MW & 9 { 5,2 9 ) { 4, 3 } cm cm , 896cm , 1326cm cm -1 Far-IR 22µm 11µm 7.6µm 5.8µm Improved line positions & intensities at 11 µm ( 5 and 2 9 bands): Coherence in the HNO 3 line intensities for the 11µm 7.6 µm 5.8 µm Perrin, Orphal, Flaud, Klee, Mellau, Mäder, Walbrodt & Winnewisser, i J. Mol. Spect 228 (2004) Flaud, Brizzi, Carlotti, A.Perrin: Perrin & Ridolfi Ohio-State Atmos. 67th Chem. Molecular Phys., Symposium, 6, 1 12, June 2012 Tran, Brizzi Gomez, Perrin, Hase, Ridolfi, Hartmann, JQSRT 110, (2009). Gomez, Tran, Perrin, Gamache, Laraia, Orphal, Chelin, Fellows, Hartmann JQSRT 110, (2009).

4 900 cm µm 1300 cm µm 1700 cm µm ACE-FTS

5 900 cm µm 1300 cm µm 1700 cm µm ACE-FTS Difference between the two profiles (900 cm -1 and 1700cm -1 bands) M. A. Wolff, Validation of HNO 3, ClONO 2, and N 2 O 5 from the the ACE-FTS spectrometer. Atmos. Chem. Phys., 8, , 2008

6 Only ONE source for the line positions & relative intensities parameters for HNO µm in the HITRAN or GEISA databases

7 Only ONE source for the line positions & relative intensities parameters for HNO µm in the HITRAN or GEISA databases Perrin, Lado-Bordowski d and dvalentin, «The 3 3 and 4 4 bands of HNO 3».Mol. Phys 67 p249 (1989) Perrin, et al. «Line intensities in the 11µm & 7.6 µm bands of HNO 3» J. Mol; Spectrosc. 160, p524 (1993)

8 Only ONE source for the line positions & relative intensities parameters for HNO µm in the HITRAN or GEISA databases Perrin, Lado-Bordowski d and dvalentin, «The 3 3 and 4 4 bands of HNO 3».Mol. Phys 67 p249 (1989) Perrin, et al. «Line intensities in the 11µm & 7.6 µm bands of HNO 3» J. Mol; Spectrosc. 160, p524 (1993) The HITRAN or GEISA updates of HNO3@7.6 µm concern only the total band intensity. Flaud, Bi Brizzi, i Carlotti, Perrin, and Ridolfi. MIPAS database: Validation of HNO 3 line parameters Atmos. Chem. Phys., 6, 1 12, 2006

9 Only ONE source for the line positions & relative intensities parameters for the HITRAN or GEISA databases Perrin, Lado-Bordowski d and dvalentin, «The 3 3 and 4 4 bands of HNO 3».Mol. Phys 67 p249 (1989) Perrin, et al. «Line intensities in the 11µm & 7.6 µm bands of HNO 3» J. Mol; Spectrosc. 160, p524 (1993) In 2011 Geoffrey Toon (JPL laboratory) evaluated the HNO 3 linelist in 7.6 µm by using it to fit the JPL MkIV balloon spectra and PNNL laboratory spectra. PNNL spectra: Chackerian, Sharpe & Blake JQSRT, 82, , 2003.

10 Geoffrey Toon powerpoint presentation PNNL spectra MkIV balloon born spectra

11 7.6 µm( 3 & 4 bands) in 1989 Only a partial analysis of the 3 and 4 bands was performed 1303 cm cm W Anh +C 3 1 Anh +C W The model did not account from the resonances involving the dark bands A.Perrin, O.Lado-Bordowski, & A. Valentin, Mol. Phys. 67, 249 (1989). Line position calculation: the calculated l energy levelsl were replaced A.Perrin: Ohio-State 67th Molecular Symposium, June 2012 by the observed ones (when existing)

12 This work FTS spectra recorded at Giessen (Germany) Bruker- 120HR in 2003 (7.6 µm) (1) FTS spectra recorded at Denver University (USA) for the hot band 12 µm (2) FTS spectra recorded at Orsay for the hot band 11 µm (3) Investigation of the PNNL HNO 3 cross sections (Pacific Northwest t National Laboratory)(4) Analyses of these spectra: New theoretical model (1)Perrin, Orphal,Flaud, Klee, Mellau,Mäder,Walbrodt,& Winnewisser, J. Mol. Spect 228 (2004) (2) Perrin, Flaud, Camy-Peyret, Winnewisser, Klee, Goldman, Murcray, Blatherwick, Bonomo, Murcray, J. Mol. Spectrosc. 166 (1994) (3) Flaud, Perrin; Orphal, Kou, Flaud, Dutkiewicz, Piccolo, JQSRT 77 (2003) A.Perrin: Ohio-State 67th Molecular Symposium, June 2012 (4) Chackerian; Sharpe, & Blake, JQSRT 82 (2003)

13 µm( 3 & 4 bands) in 2012 Two bright bands ( 3 & 4 ) four dark interacting bands.. (3 9, 2 6, & ) From the analysis of all investigated spectra: the number of assigned energy levels {3 1,4 1, 9 3, , 6 2, } is multiplied by a factor of ~2 as compared to the 1989 study A.Perrin: ASA-HITRAN 2012

14 Hamiltonian matrix A.Perrin: ASA-HITRAN 2012

15 Informations on the: * dark state from the Q branch of the hot band A.Perrin: ASA-HITRAN

16 Position of the dark band (center at cm -1 ) from the hot band Obs Orsay, 2003 (3) Flaud, Perrin; Orphal, Kou, Flaud, Dutkiewicz, Piccolo, JQSRT 77 (2003)

17 .3 9 Hamiltonian matrix E v = (cm -1 ) sym: A' A" A' A' A" A" W Fermi+C Fermi+C 9 3 W+Torsion B B strong Fermi 4 1 Fermi+C B W Anh 3 1 Fermi+C B Anh W A+B A+B strong Fermi A+B A+B W A+B A+B A+B W Informations on the: 9 3 dark state from the hot band 9 9 Large amplitude OH torsion

18 O O N O H 9 torsion OH/NO 2 (3 9 at cm -1 ) x O x H O H B N O N z y O y O z 9 torsion of OH /NO 2 large amplitude A.Perrin: Splitting Ohio-State of 62th ~ Molecular 0.06 cm Symposium, -1 in 9June

19 Obs Denver 1994 A.Perrin: Ohio-State 67th Molecular Symposium, June 2012 (2) Perrin, Flaud, Camy-Peyret, Winnewisser, Klee, Goldman, Murcray, Blatherwick, Bonomo, Murcray, J. Mol. Spectrosc. 166 (1994)

20 Transfert of the torsional splitting via the interaction Giessen 2003 A.Perrin: Ohio-State 67th Molecular Symposium, June 2012

21 Geoffrey Toon powerpoint presentation PNNL spectra MkIV balloon born spectra

22 Laboratory FTS spectrum (Univ. Giessen) Near 1320 cm -1 Spectre FTS de laboratoire (Univ. Giessen) A.Perrin ASA-HITRAN 2012

23 Laboratory FTS spectrum (Univ. Giessen) Near 1320 cm -1 Spectre FTS de laboratoire (Univ. Giessen) July 2012

24 Validation using MIPAS spectra A.Perrin: ASA-HITRAN 2012

25 HNO 3 detection by MIPAS at 1321 cm -1 MIPAS orbit 2081, July 2002, cm -1 resolution Obs HITRAN-GEISA NEW Obs-Calc HITRAN-GEISA NEW A.Perrin, ASA-HITRAN 2012

26 Geoffrey Toon powerpoint presentation PNNL spectra MkIV balloon born spectra

27 A.Perrin: Ohio-State 67th Molecular Symposium, June 2012

28 A.Perrin: ASA-HITRAN 2012

29 MIPAS orbit 2081, July 2002, cm -1 resolution Obs HITRAN NEW Obs-Calc HITRAN NEW A.Perrin: Ohio-State 67th Molecular Symposium, June 2012

30 Geoffrey Toon powerpoint presentation PNNL spectra MkIV balloon born spectra

31 Obs (Giessen, 2003)

32 Calc. 3 4 bands 2012 Obs (Giessen, 2003)

33 MIPAS orbit 2081, July 2002, cm -1 resolution Obs HITRAN NEW Obs-Calc HITRAN NEW A.Perrin: ASA-HITRAN 2012

34 What has still to be done: Try to get better fit for the line positions (if possible!!) Getting «absolute intensities» for all spectral ranges of the 3 & 4 bands at 7.6 µm Getting consistent t intensities iti for the 11 µm 7.6 µm 5.8 µm bands of HNO 3 I need high resolution data for HNO 3 for several infrared bands of HNO 3. ( band 3551 cm cm -1, 2 2 band@2645cm -1, etc..please contact me! A.Perrin: Ohio-State 67th Molecular Symposium, June 2012

35 CONCLUSION A new study of the 3 et 4 bands of HNO 3 was performed It is necessary to account for resonances involving the 3 9, 2 6 et & dark bands. I need high resolution data for HNO 3. PLEASE CONTACT ME!!!!!!!!!!!! Financial support from the French program «LEFE- CHAT» (Les Enveloppes Fluides et l'environnement, Chimie Atmosphérique) of CNRS-INSU is gratefully A.Perrin: Ohio-State 67th Molecular Symposium, June 2012 acknowledged.

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