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\title{SI TRACEABLE SATURATED ABSORPTION SPECTROSCOPY OF OZONE AT THE 50 KHZ LEVEL USING A QUANTUM CASCADE LASER AT 9.5 MICROMETRE}

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\author{\FirstName N. \LastName CAHUZAC} \address{LERMA, Sorbonne Universit\'{e}, Observatoire de Paris, PSL Universit\'{e}, CNRS, FRANCE;
LPL, Universit\'{e} Sorbonne Paris Nord, CNRS, FRANCE}

\author{\FirstName H. \LastName ELANDALOUSSI, \FirstName M. \LastName LEULIET, \FirstName P. \LastName MARIE-JEANNE, \FirstName C. \LastName ROUILL\'{E}, \FirstName T. \LastName ZANON-WILLETTE, \underline{\FirstName C. \LastName JANSSEN}}
\address{LERMA, Sorbonne Universit\'{e}, Observatoire de Paris, PSL Universit\'{e}, CNRS, FRANCE}

\author{\FirstName M. \LastName MANCEAU, \FirstName O. \LastName LOPEZ,  \FirstName B. \LastName DARQUI\'{E}}
\address{LPL, Universit\'{e} Sorbonne Paris Nord, CNRS, FRANCE}

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\author{\FirstName M. \LastName ABGRALL}
\address{LNE-SYRTE, Sorbonne Universit\'{e}, Observatoire de Paris, PSL Universit\'{e}, CNRS, FRANCE}

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\fancyhead[C]{{\footnotesize \textit{HRMS, 28th Colloquium, Dijon, France,
  Aug. 28 - Sept. 1, 2023}}}
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\category {15,9}
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Significant progress on the quantitative spectroscopy of ozone in the UV\footnote{\href{http://dx.doi.org/10.1088/1681-7575/ab0bdd}{doi:10.1088/1681-7575/ab0bdd},
J.~T. Hodges, J.~Viallon, et~al. Recommendation of a consensus value of the ozone absorption cross-section at 253.65{\hspace{0.167em}}nm based on a literature review, Metrologia \textbf{56}, 034001 (2019).}$^,$\footnote{\href{http://dx.doi.org/10.5194/amt-11-1707-2018}{doi:10.5194/amt-11-1707-2018}, C.~Janssen, H.~Elandaloussi, J.~Gr\"obner, A new photometric ozone reference in the {Huggins} bands: the
  absolute ozone absorption cross section at the 325\,nm {HeCd} laser
  wavelength, Atmos. Meas. Tech. \textbf{11}, 1707--1723 (2018).}$^,$\footnote{\href{http://dx.doi.org/10.5194/amt-13-5845-2020}{doi:10.5194/amt-13-5845-2020}, J.~Bak, X.~Liu, M.~Birk, G.~Wagner, I.~E. Gordon, K.~Chance, Impact of using a new ultraviolet ozone absorption cross-section dataset on {OMI} ozone profile retrievals, Atmos. Meas. Tech. \textbf{13}, 5845--5854 (2020).}
 and the IR\footnote{\href{http://dx.doi.org/10.1016/j.jqsrt.2021.107949}{doi:10.1016/j.jqsrt.2021.107949}, 
I.~Gordon, L.~Rothman, et~al. The {HITRAN2020} molecular spectroscopic database, J. Quant. Spectrosc. Radiat. Transfer 277, 107949 (2022).}%
$^,$\footnote{\href{http://dx.doi.org/10.1016/j.jqsrt.2021.108051}{doi:10.1016/j.jqsrt.2021.108051}, C.~Janssen, C.~Boursier, et~al. Multi-spectral investigation of ozone: {Part I. Setup} \& uncertainty budget, J. Quant. Spectrosc. Radiat. Transfer \textbf{279}, 108051 (2022).}%
$^,$\footnote{\href{http://dx.doi.org/10.1016/j.jqsrt.2021.108050}{doi:10.1016/j.jqsrt.2021.108050}, D.~Jacquemart, C.~Boursier, H.~Elandaloussi, P.~Jeseck, Y.~T{\'e}, C.~Janssen., Multi-spectral investigation of ozone: {Part II. Line} intensity measurements at one percent accuracy around 5 {$\mu$}m and 10 {$\mu$}m, J. Quant. Spectrosc. Radiat. Transfer \textbf{279}, 108050 (2022).}%
$^,$\footnote{\href{http://dx.doi.org/10.1063/1.5089134}{doi:10.1063/1.5089134}, V.~G. Tyuterev, A.~Barbe, D.~Jacquemart, C.~Janssen, S.~N. Mikhailenko, E.~N. Starikova, Ab initio predictions and laboratory validation for consistent ozone intensities in the {MW}, 10 and 5 $\mu$m ranges, J. Chem. Phys. \textbf{150} (2019).}%
$^,$\footnote{\href{http://dx.doi.org/https://doi.org/10.1016/j.jqsrt.2021.107801}{doi:10.1016/j.jqsrt.2021.107801}, V.~Tyuterev, A.~Barbe, S.~Mikhailenko, E.~Starikova, Y.~Babikov, Towards the intensity consistency of the ozone bands in the infrared range: Ab initio corrections to the S\&MPO database, J. Quant. Spectrosc. Radiat. Transfer \textbf{272}, 107801 (2021).}
has been made recently, addressing the long-standing issue of the missing consistency between UV and IR spectroscopic data for the remote sensing of ozone.\footnote{\href{https://dx.doi.org/10.1021/jp0405411}{doi:10.1021/jp0405411}, B.~Picquet-Varrault, J.~Orphal, J.-F. Doussin, P.~Carlier, J.-M. Flaud, Intercomparison of the ozone absorption coefficients in the mid-infrared (10 $\mu$m) and ultraviolet (300-350 nm) spectral regions, J. Phys. Chem. A \textbf{109}, 1008 -- 1014 (2005).} However, some uncertainty remains whether these improvements suffice to account for the striking observation of opposite trends in the global tropospheric ozone burden derived from satellite instruments (e.g. OMI or TROPOMI operating in the UV versus IASI in the IR)\footnote{\href{http://dx.doi.org/10.1525/elementa.291}{doi:10.1525/elementa.291}, A.~Gaudel, O.~R. Cooper, et~al. Tropospheric ozone assessment report: Present-day distribution and trends of tropospheric ozone relevant to climate and global atmospheric chemistry model evaluation, Elementa: Sci. Anthrop. \textbf{6} (2018).} or for the inconsistencies in the ozone retrieval from different IR bands using the same instrument.\footnote{\href{http://dx.doi.org/10.5194/amt-16-1443-2023}{doi:10.5194/amt-16-1443-2023},
M.~Kiefer, T.~von Clarmann, et~al. Version {8 IMK--IAA MIPAS} ozone profiles: nominal observation mode, Atmos. Meas. Tech. \textbf{16}, 1443--1460 (2023).} Unresolved issues in the IR spectral region at 9.5\,$\mu$m are uncertainties and inconsistencies in current ozone broadening\footnote{\href{http://dx.doi.org/10.5194/amt-11-4707-2018}{doi:10.5194/amt-11-4707-2018},
N.~Glatthor, T.~von Clarmann, G.~P. Stiller, M.~Kiefer, A.~Laeng, B.~M. Dinelli, G.~Wetzel, J.~Orphal, Differences in ozone retrieval in {MIPAS} channels {A} and {AB}: a spectroscopic issue, Atmos. Meas. Tech. \textbf{11}, 4707--4723 (2018).} and pressure shift\footnote{\href{http://dx.doi.org/10.1016/j.jms.2017.12.009}{doi:10.1016/j.jms.2017.12.009}
M.~Minissale, T.~Zanon-Willette, P.~Jeseck, C.~Boursier, C.~Janssen. First pressure shift measurement of ozone molecular lines at 9.54\,$\mu$m using a tunable quantum cascade laser. J. Molec. Spectrosc. \textbf{348}, 103--113 (2018).} parameters, as well as the question of appropriately representing molecular line shapes.\footnote{\href{http://dx.doi.org/https://doi.org/10.1016/j.jqsrt.2010.04.002}{doi:10.1016/j.jqsrt.2010.04.002}, H.~Tran, F.~Rohart, C.~Boone, M.~Eremenko, F.~Hase, P.~Bernath, J.-M. Hartmann, {Non-Voigt} line-shape effects on retrievals of atmospheric ozone: {Collisionally} isolated lines, J. Quant. Spectrosc. Radiat. Transfer \textbf{111}, 2012--2020 (2010).} % 
 These issues are best investigated using SI traceable instrumentation which provides spectral resolution surpassing that of typical high resolution Fourier transform spectrometers.


Based on previous work at LPL,\footnote{\href{http://dx.doi.org/10.1364/optica.6.000411}{doi:10.1364/optica.6.000411},
R.~Santagata, D.~B.~A. Tran, et~al. High-precision methanol spectroscopy with a widely tunable SI-traceable frequency-comb-based mid-infrared {QCL}, Optica \textbf{6}, 411--423 (2019).}$^,$%,
\footnote{\href{http://dx.doi.org/10.1038/nphoton.2015.93}{doi:10.1038/nphoton.2015.93},
B.~Argence, B.~Chanteau, et~al. Quantum cascade laser frequency stabilization at the {sub-Hz} level., Nature Phot. \textbf{9}, 456--460 (2015).} we have developed a new SI traceable high resolution laser spectrometer, which will be able to address these questions. A quantum cascade laser at 9.5\,$\mu$m is frequency stabilized on an optical frequency comb itself stabilized to a 1.55\,$\mu$m ultra-stable laser transmitted by fiber link through the REFIMEVE\footnote{\href{https://www.refimeve.fr/index.php/fr/}{www.revimeve.fr}} network from LNE-SYRTE. There it is measured
against primary standards, thus assuring SI traceability of the frequency measurements. As a first demonstration of the spectrometer perfomances, we report on line positions in the R-branch of the ozone $\nu_3$ band from saturated absorption spectroscopy with line center determinations at the 50 kHz level. This is almost three orders of magnitude more accurate than the current uncertainty index ($<$ 10$^{-3}$\,cm$^{-1}$) given in the HITRAN 2020 database.  

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