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FORUM  : Spectroscopy of minor constituents .

FORUM  : Spectroscopy of minor constituents. Agnés Perrin Laboratoire de Météorologie Dynamique (LMD UMR-CNRS 8539), Ecole Polytechnique Agnes.Perrin@lmd.polytechnique. fr J.M.Flaud , Jean-Marie.Flaud@lisa.u-pec.fr ( LISA-UMR7583 CNRS) UPE-Créteil & UPD , France. Overview.

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FORUM  : Spectroscopy of minor constituents .

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  1. FORUM :Spectroscopyof minor constituents. Agnés Perrin Laboratoire de Météorologie Dynamique (LMD UMR-CNRS 8539), Ecole Polytechnique Agnes.Perrin@lmd.polytechnique.fr J.M.Flaud, Jean-Marie.Flaud@lisa.u-pec.fr (LISA-UMR7583 CNRS) UPE-Créteil & UPD , France

  2. Overview Whatcanwe do for thisFORUMproject ? Molecules of first priority for FORUM Introduction: Who are we ? What are we able to do ? Reactive trace species to beconsidered in case of bush fires Are we able to producespectroscopicparameters for FORUM?

  3. Overview Whatcanwe do for thisFORUMproject ? Molecules of first priority for FORUM Introduction: Who are we ? What are we able to do ? Reactive trace species to beconsidered in case of bush fires Are we able to producespectroscopicparameters for FORUM ?

  4. Who are we ? • We (JM Flaud& Agnès Perrin) are specialists in theoreticalmolecularspectroscopy(positions & intensities) for infraredspectra of molecules of atmosphericinterest • Jean-Marie Flaudisfrom the LISA laboratory at Creteil. • I (AP) belongs to the ABC(t) group at LMD laboratory (Ecole Polytechnique). • Raymond Armanteand myself are now responsible of the GEISA database. Some of my colleagues are well known specialists in line shape parameters (non Voigt, line mixing, continua)

  5. What are we able to do ? • For the MIPAS project, Jean-Marie Flaudand Marco Ridolfiare responsible of the definition of the MIPAS spectroscopic database. • I (AP) was (very) partially collaboringon the MIPAS project with Marco Ridolfi& Jean-Marie. • I was also involved in several ESA project with S.Bühler.

  6. IASI « Nouvelle Génération in 2022 ) As far as IASI-NG isconcerned, we are usingMIPAS spectra to « validate » the line by line listsfor the future IASI>NG (on going collaboration with the Bolognagroup (Marco Ridolfi)

  7. HNO3 Bad quality of the HNO3 spectroscopicparamaters at 7.6 µm IASI on METOP Preparation of IASI-NewGeneration(2021) MW & n9{n5,2n9){n4,n3} n2 0-10cm-1 458cm-1 879, 896cm-1 1303, 1326cm-1 1709cm-1 Far-IR 22µm 11µm 7.6µm 5.85 µm (in water) Goal for IASI -NG: to enablesimultaneousdetection of HNO3both at 11 µm & 7.6 µm usingMIPAS spectra

  8. Strategy for HNO3 11 µm &7.6 µmbands : ¤ Wekept the 11 µm band line parameters as they are in GEISA or HITRAN ¤ For the 7.6 µmregion: new linelist(betterline positions & intensities) ¤ 7.6 µmregionimproved line parametersduring a laboratoryspectroscopicanalysis(A.P. & JMF). : • Laboratoryspectrarecorded in welldefined conditions • theoretical computations of line positions & relative line intensities. ¤ Satellite validation (byM.Ridolfi@ Bologna) usingMIPASspectra: Intercalibrationof line intensitiesfor the new7.6 µm linelistrelativelyto 11 µmband

  9. New line list GEISA or HITRAN Marco Ridolfi 11 µm Not updated 7.6 µm updated A.Perrin: ISMS Molecular Symposium, June 2015

  10. ---Obs MIPAS spectrum --- Calc (NEW database) --- Calc (OLD database) M.Ridolfi & M.Carlotti --- Obs-Calc (NEW database) --- Obs-Calc (OLD database)

  11. HNO3 concentration profile (v.s. altitude) using the « old » database… 7.6 µm  11 µm Before… M.Ridolfi & M.Carlotti

  12. HNO3 concentration profile (v.s. altitude) using the « new » database… 7.6 µm  11 µm After … M.Ridolfi & M.Carlotti

  13. Overview Whatcanwe do for thisFORUMproject ? Molecules of first priority for FORUM Introduction: Who are we ? What are we able to do ? Reactive trace species to beconsidered in case of bush fires Are we able to producespectroscopicparameters for FORUM ?

  14. FORUM versus IASI-NG

  15. Several spectroscopic studies were performed recently for IASI-NG. The MIPAS (700 – 2300 cm-1) spectra Refs: see the co-authors in this room) can be « used » for the validation of the database for IASI-NG IASI-NG andFORUM MIPAS For FORUM informations are requested for (i) the molecules of troposphericinterest(whichwere not alwaysconsidered by MIPAS) (ii) « line by line » parameters are preferred (if possible) to cross sections parameters  (they lead to betteratmosphericretrievals) (iii) the line shape (and continua) for moleculespresent in the troposphereneedprecise description FORUM is covering the 150- 1400 cm-1spectral region and none of the recent satellite instruments(MIPAS, IASI or ACE-FTS) are covering the low frequency region 120 cm-1< s < 700 cm-1. We have to provide accurate spectroscopic parameters for preparing this mission

  16. Unplanned observations ???? IASI (instrument with a ratherweakresolutionR=0.5 cm-1) dedicatedfor (mainly) meteorological applications (température, humidity & eventually ozone columns) During the preparation of the IASI mission (before the launching of METOP-A in 2006) a spectroscopiclinelistwasprepared for a restrictedlist of molecules( Water, CO2, O3, N2O, CO, methane, NO ) IASI: « unplanned » observations: acidrains (formicacid, HCOOH), « NH3 global map , detection of SO2 in volcanic plumes, (cfLATMOS et ULB-Bruxelles), etc…

  17. Strategy: short review of the status of the spectroscopicparameters for molecules of interest for FORUM • Wesearch for molecules of atmosphericinterestwhich have a ratherstronginfrared signature in the spectral range of FORUM (200-1300 cm-1). • At thislevel, we do NOTtry to identify the possible interferencesof the infrared signature of thesespecieswithabsorption due to specieswithstrong IR signature (water, CO2, etc…) In this talk, I did not consider the problem of continua (water, N2-N2, O2-N2etc) or of indices (water ice…).

  18. The first investigation concernsmoleculesobserved in IASI spectra in so-called «regularconditions» (H2O, HDO, CO2, CO, CH4, O3, N2O, CO, N2O, OCS, HNO3, CFC‐11 (CCl3F), CFC‐12 (CCl2F2), and CF4 ) Can wedetectthesespecieswith FORUM ??

  19. ….second, we look for moleculesidentified in « special » conditions in IASI spectra: ….(mostly) short‐lived trace gases: sulfur dioxide (SO2), ammonia (NH3), OCS, methanol(CH3OH), formic acid (HCOOH), ethene (C2H4) and PAN (C2H3O5N) … observable above the Po valley or during Volcano eruptions … and rare reactive trace gas species … (like nitrousacid, furan, acetylene, propylene, aceticacid, formaldehyde and hydrogencyanide, acetylene ) , observable duringAustralian bush fires of February 2009.

  20. Overview Whatcanwe do for thisFORUMproject ? Molecules of first priority for FORUM Except for Water & associated continua (S.Buëhler , E.Hegglin, M. Mlawer) Water & CO2spectroscopy (C.Serio et al. ) Introduction: Who are we ? What are we able to do ? Reactive trace species to beconsidered in case of bush fires Are we able to producespectroscopicparameters for FORUM ?

  21. Moleculeswhich do not have a stronginfrared signature in the FORUM spectral range . CO, O2, N2, NO, OH, HF, HCl, HI: => not relevant • OCS (carbonylsulfide) • Strongest signature is at 2062 cm-1 (not usable by FORUM ) compared to IASI-NG ! • For details: seeCamy-Peyret, Liuzzi, Masiello, Serio, Venafra, Montzka, JQSRT 201 (2017) 197-208

  22.  Probably not observable by FORUM • Nitrousoxide (N2O) For N2O: Band n2 (589cm-1) , n3 (1285 cm-1) ,n1 (2224 cm-1) Intensities ratio: 0.10 / 1. / 5.7 in 10-17cm-1 cm-1/(molecule.cm-2) • Nitrogendioxide: NO2 Evidence of line mixing effets (see C. Camy-Peyret for details) -------------------------------------------------------------------------------------------------------------------------------------------------------- sameinfrared signature as IASI-NG For NO2: Band n2 (750) , n1 (1320 cm-1) , n3 (1617 cm-1) Intensities ~ 0.57 / 0.005 / 5.8 in 10-17cm-1/(molecule.cm-2)

  23. sameinfrared signature as for IASI-NG Ozone (O3) For 16O3: Band n2 (700.93) , n3 (1042.08 cm-1) n1 (1103.14 cm-1) Intensities: 0.59 14.1 0.54 in 10-18.cm-1/(molecule.cm-2) Q: Check the relative intensityof the n2band versus the {n3n1 } interacting bands

  24. Methane: (seeLiuzziet al 2016) Sameinfrared signature as IASI-NG (seeLiuzziet al. 2016) • For the n4 Q branch: intense spike at 1306 cm-1 in IASI spectra From: Liuzzi, Masiello, Serio, Venafra, Camy-Peyret JQSRT 182 (2016) 128

  25. . Ammonia (NH3)=> n2region (at 10 µm) like for IASI Sameinfrared signature as IASI-NG Check the spectroscopybecause of the importance of ammonia for the pollution by NH3 in the Po valley 800 900 1000 1100 1200 cm-1

  26. Nitricacid (HNO3) For MIPAS, IASI or ACE-FTS Overlapped by water

  27. C-type band Nitric acid (HNO3) Verysharp C-type band 1.12.0 3.7 4.4 Band Intensities 10-17cm-1/(molecule.cm-2)

  28. Is the n9 band region (22 µm) usable by FORUMfor the HNO3retrievals? 1.12.0 3.7 4.4 Band Intensities 10-17cm-1/(molecule.cm-2)

  29. Was the n9regionused by anyotherremotesensing instrument? 1.12.0 3.7 4.4 Band Intensities 10-17cm-1/(molecule.cm-2)

  30. Spectroscopic analysis Balloon flight of the FIRS-2 spectrometer from the Harvard–Smithsonian Center for Astrophysics…. thermal emission spectra taken at a resolution of 0.004 cm−1.

  31. HNO3: spectroscopicproblems for (1) Internalconsistencyof the line intensitiesfor the 22 µm region(n9 band) relative to the 11 µm region{n5 , 2n9} bands 22 µm 11 µm

  32. HNO3: spectroscopicproblems for (2) Line mixingproblems • Werealreadyidentified in IASI spectra for the n5 band Liuzzi, Masiello, Serio, Venafra , Camy-Peyret, JQSRT 182 (2016) 128-157

  33. In laboratory conditions, line mixingeffectsalreadyobserved for several HNO3 bands for narrow Q branches of HNO3 .n8 band of HNO3 Gomez, Tran, Perrin, Gamache, Laraia, Orphal, Chelin, Fellows, Hartmann, JQSRT, 110 (2009) 675

  34. Line mixingeffects are (also) highly probable in atmosphericspectra in the Q- branch of the n9 region(22 µm)

  35. Formaldehyde (H2CO) Sameinfrared signature as for IASI-NG Covered by HITRAN & GEISA Absent in HITRAN & GEISA

  36. Hypochlorousacid (HOCl) (35Cl and 37Cl) • For HO35Cl : n2 at 1238.62 cm-1 ; n3 at 724.36 cm-1 • For HO37Cl : n2 at 1238.12 cm-1 ; n3 at 718.17 cm-1 • Intensity ratio (n2/n3) ≈ 6 . The n3 band at ~720 cm-1islikelytoo weak to be usable Sameinfrared signature than for IASI-NG Lafferty & Olson, J. Mol. Spectrosc 120 (1986) 359

  37. Overview Whatcanwe do for thisFORUMproject ? Molecules of first priority for FORUM Introduction: Who are we ? What are we able to do ? Reactive trace species to beconsidered in case of bush fires Observed in IASI spectra (Australiafires) Clarisse et al. GRL 38, L10802, doi:10.1029/2011GL047271, 2011 Furan, HONO, Acetylene, HCN, … Are we able to producespectroscopicparameters for FORUM ?

  38. PAN (C2H3O5N) Sameinfrared signature than for IASI-NG Observed in IASI spectra (Australia bush fires in 2009) Clarisse et al. GRL 38, L10802, doi:10.1029/2011GL047271, 2011 PNNL cross sections. Sharpe et al. AppliedSpectroscopy 58 (2004) 1452-1461

  39. FURAN (C4H4O) PNNL cross sections. Sharpe et al. AppliedSpectroscopy 58 (2004) 1452-1461 Obviously the 743 cm-1 band is the « best region » for furandetection by FORUM and IASI-NG

  40. FURAN (C4H4O) PNNL cross sections. Sharpe et al. AppliedSpectroscopy 58 (2004) 1452-1461 must bedetected by Observed in IASI spectra (Australiafires) Clarisse et al. GRL 38, L10802, doi:10.1029/2011GL047271, 2011 Need line by line spectroscopicparameters

  41. n5 n4 PNNL cross sections of HONO (nitrousacid). Sharpe et al. AppliedSpectroscopy 58 (2004) 1452-1461

  42. n5 n4 For IASI only then4band regionis usable ! n4 HONO observed in IASI spectra (Australia bush fires in 2009) Clarisse et al. GRL 38, L10802, doi:10.1029/2011GL047271, 2011

  43. Need line by line list of spectroscopicparameters n5 n4 Good news: FORUM willpossiblydetect????? Trans-HONO and Cis-HONO in both the n4 band & n5 band regions. Perrin et al. JMS (2007) n4 HONO observed in IASI spectra (Australia bush fires in 2009) Clarisse et al. GRL 38, L10802, doi:10.1029/2011GL047271, 2011

  44. Acetylene (C2H2) ~729 cm-1 Hydrogencyanide (HCN) ~713cm-1 Formicacid (HCOOH): ~1033 cm-1 Linelist (line by line) available in HITRAN & GEISA Observed in IASI spectra (Australia bush fires in 2009) Clarisse et al. GRL 38, L10802, doi:10.1029/2011GL047271, 2011

  45. Overview Whatcanwe do for thisFORUMproject ? Molecules of first priority for FORUM Reactive trace species to beconsidered in case of bush fires Are we able to producespectroscopicparameters for FORUM ? Introduction: Who are we ? What are we able to do ? Weneed good qualitylaboratoryspectra in the 150 – 1400 cm-1 spectral range We have a large experiencein theoreticalmodelsfor line positions and intensities for numerousmolecularspecies

  46. We are working in close contact with high qualifiedexperimentalspectroscopists (L.Manceron, F.Kwabia)

  47. Upper trace: liquid nitrogen cooled D316 commercial detector, shifted one unit of transmission. SOLEIL-MCT detector at 4 K. The gain in RMS S/N ratio varies here from about 12 to 6 from one end to the other of the spectrum. Comparison of two spectra taken at identical experimental conditions for the ν2 region of CO2 in 5 mb of air with a resolution of 0.002 cm−1, 42 min recording time, APT = 2 mm, and KBr/Ge beam splitter. Mbaye Faye, Bordessoule, Kanouté,Brubach, Roy, Manceron, Rev of Scient. Inst. 87, 063119 (2016)

  48. Conclusion • We presented a short overview of the status of the spectroscopic parameters for the molecules of interest for FORUM • This review concerns molecules of “first priority” and also molecules which may possibly be detected in case of “unusual conditions” in for FORUM atmospheric spectra • We are ready to produce the spectroscopic parameters to help these detections by FORUM

  49. Continua ????(new CIA section of the HITRAN database) O2-O2

  50. Balloon flight of the FIRS-2 spectrometer from the Harvard–Smithsonian Center for Astrophysics[Petkie, et al (K.W. Jucks) JQSRT 92 (2005) 129–141 The FIRS-2 balloon spectrum of the v5–v9 and 2v9–v9 regions along with radiative transfer simulations of the bands. Upper solid trace: observed balloon spectrum Dashed trace is the simulated spectrum Lower solid line is the residual (observed–simulated). Limb viewing geometry with balloon altitude of 37 km and a tangent altitude of 20 km.

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