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  <front>
    <journal-meta><journal-id journal-id-type="publisher">ACP</journal-id><journal-title-group>
    <journal-title>Atmospheric Chemistry and Physics</journal-title>
    <abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys.</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">1680-7324</issn><publisher>
    <publisher-name>Copernicus Publications</publisher-name>
    <publisher-loc>Göttingen, Germany</publisher-loc>
  </publisher></journal-meta>
    <article-meta>
      <article-id pub-id-type="doi">10.5194/acp-18-6939-2018</article-id><title-group><article-title>Multi-year assimilation of IASI and MLS ozone retrievals:
variability of tropospheric ozone over the tropics<?xmltex \hack{\newline}?> in response
to ENSO</article-title><alt-title>Tropospheric Ozone in response to ENSO</alt-title>
      </title-group><?xmltex \runningtitle{Tropospheric Ozone in response to ENSO}?><?xmltex \runningauthor{H. Peiro et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Peiro</surname><given-names>Hélène</given-names></name>
          <email>peiro@cerfacs.fr</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Emili</surname><given-names>Emanuele</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Cariolle</surname><given-names>Daniel</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Barret</surname><given-names>Brice</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Le Flochmoën</surname><given-names>Eric</given-names></name>
          
        </contrib>
        <aff id="aff1"><label>1</label><institution>CECI, Université de Toulouse, Cerfacs, CNRS, Toulouse, France</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Météo-France, Toulouse, France</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Laboratoire d'Aérologie, Université de Toulouse, CNRS, UPS, Toulouse, France</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Hélène Peiro (peiro@cerfacs.fr)</corresp></author-notes><pub-date><day>17</day><month>May</month><year>2018</year></pub-date>
      
      <volume>18</volume>
      <issue>9</issue>
      <fpage>6939</fpage><lpage>6958</lpage>
      <history>
        <date date-type="received"><day>15</day><month>September</month><year>2017</year></date>
           <date date-type="rev-request"><day>15</day><month>November</month><year>2017</year></date>
           <date date-type="rev-recd"><day>15</day><month>April</month><year>2018</year></date>
           <date date-type="accepted"><day>20</day><month>April</month><year>2018</year></date>
      </history>
      <permissions>
        
        
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018.html">This article is available from https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018.pdf</self-uri>
      <abstract>
    <p id="d1e132">The Infrared Atmospheric Sounder Instrument (IASI) allows global coverage
with very high spatial resolution and its measurements are promising for
long-term ozone monitoring. In this study, Microwave Limb Sounder (MLS) O<inline-formula><mml:math id="M1" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
profiles and IASI O<inline-formula><mml:math id="M2" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> partial columns (1013.25–345 hPa) are assimilated
in a chemistry transport model to produce 6-hourly analyses of tropospheric
ozone for 6 years (2008–2013). We have compared and evaluated the IASI-MLS
analysis and the MLS analysis to assess the added value of IASI measurements.</p>
    <p id="d1e153">The global chemical transport model MOCAGE (MOdèle de Chimie
Atmosphérique à Grande Echelle) has been used with a linear ozone
chemistry scheme and meteorological forcing fields from ERA-Interim (ECMWF
global reanalysis) with a horizontal resolution of
2<inline-formula><mml:math id="M3" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M4" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 2<inline-formula><mml:math id="M5" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> and 60 vertical levels. The MLS and IASI
O<inline-formula><mml:math id="M6" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> retrievals have been assimilated with a 4-D variational algorithm to
constrain stratospheric and tropospheric ozone respectively. The ozone
analyses are validated against ozone soundings and tropospheric column
ozone (TCO) from the OMI-MLS residual method. In addition, an Ozone ENSO
Index (OEI) is computed from the analysis to validate the TCO variability
during the ENSO events.</p>
    <p id="d1e190">We show that the assimilation of IASI reproduces the variability of
tropospheric ozone well during the period under study. The variability deduced
from the IASI-MLS analysis and the OMI-MLS measurements are similar for the
period of study. The IASI-MLS analysis can reproduce the extreme oscillation
of tropospheric ozone caused by ENSO events over the tropical Pacific Ocean,
although a correction is required to reduce a constant bias present in the
IASI-MLS analysis.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p id="d1e200">Tropospheric ozone (O<inline-formula><mml:math id="M7" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>) is the third most important greenhouse gas
<xref ref-type="bibr" rid="bib1.bibx34" id="paren.1"/>. It influences the atmospheric radiative forcing as one
of the main absorbers of infrared and ultraviolet radiation
<xref ref-type="bibr" rid="bib1.bibx78 bib1.bibx37" id="paren.2"/>. It also has a strong effect on human health and
vegetation. High levels of O<inline-formula><mml:math id="M8" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations increase pulmonary and
chronic respiratory diseases, increasing human premature mortality
<xref ref-type="bibr" rid="bib1.bibx31 bib1.bibx8 bib1.bibx25" id="paren.3"/>. High concentrations of O<inline-formula><mml:math id="M9" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> reduce
photosynthesis and other important physiological functions of vegetation
<xref ref-type="bibr" rid="bib1.bibx87" id="paren.4"/>. Due to its relatively long lifetime (<inline-formula><mml:math id="M10" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 2 weeks in
the troposphere), the global variability of tropospheric ozone is the
combination of the complex interactions between anthropogenic emissions,
chemical production and destruction, long-range transport, and
stratosphere–troposphere exchanges. A global increase in tropospheric ozone
has been documented during the last 30 years <xref ref-type="bibr" rid="bib1.bibx17" id="paren.5"/>, the cause of
which is not yet well understood <xref ref-type="bibr" rid="bib1.bibx28" id="paren.6"/>. To determine the
origin of this trend, it is important to evaluate the relative contributions
between natural variability and anthropogenic forcing.</p>
      <?pagebreak page6940?><p id="d1e256">Among the natural forcings, the El Niño Southern Oscillation (ENSO) is an
atmospheric phenomenon with a large-scale circulation pattern that influences
the O<inline-formula><mml:math id="M11" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> distribution <xref ref-type="bibr" rid="bib1.bibx12 bib1.bibx88" id="paren.7"/> with a periodicity of
about 2–7 years. ENSO refers to two events in the tropical Eastern Pacific:
El Niño (anomalously warm ocean temperatures) and La Niña
(anomalously cold ocean temperatures). ENSO is the dominant source of the
tropical Pacific variability for the atmosphere and the ocean
<xref ref-type="bibr" rid="bib1.bibx77 bib1.bibx57" id="paren.8"/>. During ENSO, changes in sea-surface
temperatures (SSTs) in the Pacific Ocean have a large influence on the normal
atmospheric circulation, displacing the location of convection and its
intensity <xref ref-type="bibr" rid="bib1.bibx59" id="paren.9"/>. These changes in circulation impact the
temperature and moisture fields across the tropical Pacific, influencing the
chemical composition of the troposphere (<xref ref-type="bibr" rid="bib1.bibx94" id="altparen.10"/>;
<xref ref-type="bibr" rid="bib1.bibx60" id="altparen.11"/>, Fig. <xref ref-type="fig" rid="Ch1.F1"/>).</p>
      <p id="d1e286">Convection during ENSO affects tropical tropospheric O<inline-formula><mml:math id="M12" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> in two ways.
First, convection impacts the vertical mixing of O<inline-formula><mml:math id="M13" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> itself. Convection
lifts lower tropospheric air masses with a low ozone concentration, where
O<inline-formula><mml:math id="M14" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> lifetime is shorter, to upper troposphere where O<inline-formula><mml:math id="M15" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> lifetime is
longer <xref ref-type="bibr" rid="bib1.bibx21" id="paren.12"/>. Overall increased convection leads to a decrease
in the tropospheric ozone column (Fig. <xref ref-type="fig" rid="Ch1.F1"/>a). Second, convection
affects vertical mixing and vertical distribution of O<inline-formula><mml:math id="M16" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> precursors
<xref ref-type="bibr" rid="bib1.bibx70" id="paren.13"/>. El Niño events coincide with dry conditions
generating large-scale biomass burning in Indonesia <xref ref-type="bibr" rid="bib1.bibx13" id="paren.14"/>.
During El Niño, TCO over Indonesia is higher than average. A remarkable
change in the tropospheric O<inline-formula><mml:math id="M17" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentration due to El Niño occurred in
the western part of Pacific during 1997–1998, with an increase in the TCO of
<inline-formula><mml:math id="M18" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>20 to <inline-formula><mml:math id="M19" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>25 DU <xref ref-type="bibr" rid="bib1.bibx13" id="paren.15"/>. Atmospheric particulates and O<inline-formula><mml:math id="M20" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
precursors increase in Indonesia (Fig. <xref ref-type="fig" rid="Ch1.F1"/>b). During La Niña
events, dry conditions are located in South America, causing an increase of TCO
in the eastern Pacific Ocean (Fig. <xref ref-type="fig" rid="Ch1.F1"/>c).</p>

      <?xmltex \floatpos{p}?><fig id="Ch1.F1"><caption><p id="d1e388">Schematic of the Walker circulation over the Pacific
ocean. <bold>(a)</bold> During normal conditions: trade winds induce subsidence
along South America with intrusion of O<inline-formula><mml:math id="M21" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>-rich air. The TCO is elevated. In
addition, along Indonesia, warmer waters generate convergence that results in
low O<inline-formula><mml:math id="M22" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations. The TCO is weakened <bold>(b)</bold> during El
Niño events: easterly trade winds are weakened. Therefore, convergence
areas are located near the coast of South America while subsidence zones are
located in the Indonesia. Low TCO is located over the Pacific ocean while
high TCO is located over Indonesia, and <bold>(c)</bold> during La Niña
events: during exceptionally strong trade winds the convergence over the
Indonesia is stronger. The TCO has the lowest value. Subsidence over South
America brings air masses with high O<inline-formula><mml:math id="M23" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentration, resulting in higher
TCO than average values.</p></caption>
        <?xmltex \igopts{width=233.312598pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018-f01.png"/>

      </fig>

      <p id="d1e435">Previous studies have characterized the variations of the tropical
tropospheric O<inline-formula><mml:math id="M24" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> linked to ENSO <xref ref-type="bibr" rid="bib1.bibx93" id="paren.16"/>. To characterize the
ENSO amplitude several ENSO indices have been proposed based on ENSO
footprints on the pressure field or the outgoing longwave radiation
<xref ref-type="bibr" rid="bib1.bibx2 bib1.bibx77" id="paren.17"/>. <xref ref-type="bibr" rid="bib1.bibx91" id="text.18"/> developed such an index
for Ozone, the Ozone ENSO Index (OEI), to better characterize the effect of
the oscillation on the O<inline-formula><mml:math id="M25" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> distribution and as a diagnostic tool for
tropospheric chemistry models.</p>
      <?pagebreak page6941?><p id="d1e465">A detailed analysis of the effects of convection on tropospheric O<inline-formula><mml:math id="M26" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> has
been prevented so far by the paucity of observations
<xref ref-type="bibr" rid="bib1.bibx69 bib1.bibx38" id="paren.19"/>. The restricted number of ozonesonde
observations limits analysis of the links between O<inline-formula><mml:math id="M27" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and ENSO
<xref ref-type="bibr" rid="bib1.bibx74" id="paren.20"/>. Satellite observations can give more information on
the O<inline-formula><mml:math id="M28" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> variability, and their global coverage gives better insight into the
processes involved in ENSO <xref ref-type="bibr" rid="bib1.bibx91" id="paren.21"/>. To derive tropospheric O<inline-formula><mml:math id="M29" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
several studies have combined ozone measurements from the Ozone Monitoring
Instrument (OMI) that measures the total ozone columns, and the Microwave
Limb Sounder (MLS) that provides vertical ozone profiles in the upper
troposphere and stratosphere. <xref ref-type="bibr" rid="bib1.bibx90" id="text.22"/> subtracted the stratospheric
column O<inline-formula><mml:math id="M30" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> (of MLS) from the total column O<inline-formula><mml:math id="M31" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> (of OMI) to obtain the
tropospheric column O<inline-formula><mml:math id="M32" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> (named hereafter OMI-MLS). They show a large impact
of ENSO on tropospheric O<inline-formula><mml:math id="M33" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> in the tropics by analyzing the OMI-MLS data
<xref ref-type="bibr" rid="bib1.bibx93" id="paren.23"/>. The O<inline-formula><mml:math id="M34" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> sensitivity to ENSO was also studied with the
tropospheric emission spectrometer (TES) observations <xref ref-type="bibr" rid="bib1.bibx51" id="paren.24"/>. They
studied, during El Niño, the long-range transport of Asian pollution due
to the Northern Hemisphere subtropical jet. MLS and TES data were also
compared to a chemistry–climate model to study how ENSO can influence the
O<inline-formula><mml:math id="M35" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> distribution <xref ref-type="bibr" rid="bib1.bibx55" id="paren.25"/>. These studies demonstrate that the link
between O<inline-formula><mml:math id="M36" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and ENSO becomes a key element of the chemistry–climate
interactions.</p>
      <p id="d1e591">The combination of OMI and MLS measurements allows insights into the links
between tropospheric O<inline-formula><mml:math id="M37" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and ENSO, but has limitations because the
tropospheric partial O<inline-formula><mml:math id="M38" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> columns are obtained as a difference between two
large quantities, the total column and the stratospheric column. Hence,
possible bias and errors in MLS and OMI data can be amplified when the
partial tropospheric column is calculated. The objective of the present study
is to obtain direct evaluations of tropospheric ozone using assimilation of
ozone profiles from MLS and from IASI.</p>
      <p id="d1e612">The IASI instrument, launched onboard MetOp-A in 2006, was designed for
numerical weather predictions and atmospheric composition observations
<xref ref-type="bibr" rid="bib1.bibx15" id="paren.26"/>. IASI allows a daily global coverage at very high
spatial resolution (12 km for nadir observations). Because of its spatial
coverage, the day and night retrieval coverage, IASI provides an important
added value with respect to other satellites like TES or OMI
<xref ref-type="bibr" rid="bib1.bibx32 bib1.bibx58 bib1.bibx52" id="paren.27"/>. The IASI mission is meant to last
for several decades (MetOp) whereas the instruments OMI, MLS and TES are
scientific missions with limited lifespan. Tropospheric O<inline-formula><mml:math id="M39" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> from IASI has
been already studied and validated. The IASI ozone data were found to be
particularly well suited to the study of O<inline-formula><mml:math id="M40" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> variations in the upper troposphere
<xref ref-type="bibr" rid="bib1.bibx24 bib1.bibx75 bib1.bibx7" id="paren.28"/>. Since we already have about 10
years of data, the IASI mission provides a valuable dataset to study the
O<inline-formula><mml:math id="M41" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> variability and trends <xref ref-type="bibr" rid="bib1.bibx76 bib1.bibx84" id="paren.29"/>, both in the
troposphere and the stratosphere
<xref ref-type="bibr" rid="bib1.bibx82 bib1.bibx83 bib1.bibx23 bib1.bibx6 bib1.bibx64 bib1.bibx61" id="paren.30"/>.
More recently, the tropospheric O<inline-formula><mml:math id="M42" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> variability due to ENSO has been
studied using 8 years (January 2008 to March 2016) of IASI measurements
<xref ref-type="bibr" rid="bib1.bibx85" id="paren.31"/>. They have shown that IASI retrievals can capture the
variability of tropospheric ozone related to the large-scale dynamical modes
of ENSO.</p>
      <p id="d1e670">By assimilating IASI data within the MOCAGE model <xref ref-type="bibr" rid="bib1.bibx73" id="paren.32"/>, we
expect to obtain O<inline-formula><mml:math id="M43" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> distributions consistent with OMI-MLS observations and
to have additional information on the vertical O<inline-formula><mml:math id="M44" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> distributions in the
troposphere. We use the MOCAGE chemistry transport model (CTM) to assimilate
tropospheric ozone profiles from IASI and stratospheric profiles from MLS
with a 4D-Var (4-dimensional-variational) algorithm. The joint assimilation
of IASI and MLS data was already found to improve modeled O<inline-formula><mml:math id="M45" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> in the UTLS
<xref ref-type="bibr" rid="bib1.bibx5 bib1.bibx27" id="paren.33"/>. Since the information in IASI retrievals is
strongly weighted in the troposphere, the assimilation of MLS allows the
introduction of complementary information in the case of
stratosphere–troposphere exchanges <xref ref-type="bibr" rid="bib1.bibx4" id="paren.34"/>, which intensify over
the eastern Pacific Ocean during the La Niña phase of the ENSO. We will
evaluate in this study the relative importance of assimilating MLS and IASI
in the context of the O<inline-formula><mml:math id="M46" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> variability related to ENSO. To compute ozone
tendencies MOCAGE uses the latest version of the linear ozone chemistry
parametrization of <xref ref-type="bibr" rid="bib1.bibx11" id="author.35"/> (CARIOLLE Scheme,
<xref ref-type="bibr" rid="bib1.bibx11" id="year.36"/>).</p>
      <p id="d1e725">The influence of ENSO on tropical tropospheric O<inline-formula><mml:math id="M47" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> has been simulated by
CTMs or by global chemistry–climate models
<xref ref-type="bibr" rid="bib1.bibx72 bib1.bibx88 bib1.bibx22 bib1.bibx54" id="paren.37"/>. Fewer studies used
data assimilation to study the distribution and interannual variability of
tropospheric ozone in the Pacific <xref ref-type="bibr" rid="bib1.bibx41 bib1.bibx53" id="paren.38"/>. Data
assimilation allows time series of chemical fields that integrate
all available information from measurements and models to be obtained. This can be
particularly useful when tropospheric retrievals from satellite measurements
become very sparse, due for instance to the occurrence of convective clouds
in the tropical region. Furthermore, the assimilation of IASI data for a long
time period has not yet been considered. The 6-year reanalysis
(2008–2013) of tropospheric O<inline-formula><mml:math id="M48" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> that we have computed in the present study
is ideal for studying the ozone variability in the tropics from short-term to
interannual timescales.</p>
      <p id="d1e753">The format of this paper is as follows. In Sect. 2 we describe the
observations used for assimilation and model validation, as well as the settings
used by the MOCAGE model and the assimilation suite. In Sect. 3 we discuss
the results obtained assimilating IASI and MLS data, with an emphasis on the
impact of ENSO on tropospheric O<inline-formula><mml:math id="M49" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>. We derive an Ozone ENSO Index and
compare its evolution to previous studies. The final section summarizes the
results.</p>
</sec>
<sec id="Ch1.S2">
  <title>Methodology</title>
<sec id="Ch1.S2.SS1">
  <title>Assimilated observations</title>
<sec id="Ch1.S2.SS1.SSS1">
  <title>IASI and MetOp-A measurements</title>
      <p id="d1e781">The IASI is one of the instruments onboard the polar-orbiting satellite
MetOp-A (Meteorological Operational), which is operated by the European
organization for the exploitation of Meteorological Satellites (EUMETSAT).
The MetOp-A<?pagebreak page6942?> satellite was launched on 19 October 2006 and has already
provided data for about 10 years. Due to its inclination to the equatorial
plane and its altitude (817 km), MetOp-A crosses the equatorial plane at
09:30 and 21:30 LT (the equatorial plane at 9:30 and 21:30 local solar time when crossing the Equator).</p>
      <p id="d1e784">IASI is a nadir-viewing Fourier Transform Spectrometer. The detectors sense
in the thermal infrared spectral range between 645 and 2760 cm<inline-formula><mml:math id="M50" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (15.5
to 3.62 <inline-formula><mml:math id="M51" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m). IASI provides spectra with a high radiometric quality
at a resolution of 0.5 cm<inline-formula><mml:math id="M52" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (after apodization). IASI measurements are
taken along- and across-track over a swath width of 2200 km with an
horizontal resolution of 12 km. Therefore, IASI provides global coverage
twice a day. The high spectral resolution of IASI allows the retrieval of
vertical profiles of a number of gases affecting the climate system and the
atmospheric pollution <xref ref-type="bibr" rid="bib1.bibx15 bib1.bibx16" id="paren.39"/>. Previous studies have
used vertical information from IASI Level 2 products to study O<inline-formula><mml:math id="M53" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> in the
troposphere, in the upper troposphere–lower stratosphere (UTLS) and in the
stratosphere <xref ref-type="bibr" rid="bib1.bibx23 bib1.bibx6 bib1.bibx7 bib1.bibx83 bib1.bibx75" id="paren.40"/>.</p>
      <p id="d1e834">A radiative transfer code and retrieval software are used to retrieve O<inline-formula><mml:math id="M54" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
profiles from IASI radiances. We use O<inline-formula><mml:math id="M55" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> retrievals performed with the
Software for Fast Retrieval of IASI Data <xref ref-type="bibr" rid="bib1.bibx6" id="paren.41"/> developed at
Laboratoire of Aerology. The SOFRID (SOftware for a Fast Retrieval of IASI
Data) is based on the RTTOV (Radiative Transfer for TOVS,
<xref ref-type="bibr" rid="bib1.bibx62 bib1.bibx63" id="altparen.42"/>) fast radiative transfer
model coupled to the 1D-Var algorithm developed at UKMO (United Kingdom Met
Office, <xref ref-type="bibr" rid="bib1.bibx56" id="author.43"/>, <xref ref-type="bibr" rid="bib1.bibx56" id="year.44"/>). SOFRID retrieves
the O<inline-formula><mml:math id="M56" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> profiles on 43 levels from 1013.25 to 0.1 hPa using a single a
priori profile and covariance matrix based on 1 year of in situ
observations (see <xref ref-type="bibr" rid="bib1.bibx6" id="altparen.45"/> for details). Validation of 6 months
of tropospheric O<inline-formula><mml:math id="M57" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> columns from IASI-SOFRID against ozonesondes and
airborne data have shown biases of about 5 % and relative standard
deviation (RSD) of about 15 % in the tropics. In their validation study of
three IASI O<inline-formula><mml:math id="M58" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> products over 1 year, <xref ref-type="bibr" rid="bib1.bibx24" id="text.46"/> also found biases
of 3.8 and RSD of 9.5 % for IASI-SOFRID tropospheric O<inline-formula><mml:math id="M59" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> relative to
ozonesonde data in the tropics. In this study, partial O<inline-formula><mml:math id="M60" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> columns between
1013.25 and 345 hPa has been computed from the IASI-SOFRID profile prior to
the assimilation.</p>
</sec>
<sec id="Ch1.S2.SS1.SSS2">
  <title>MLS measurements</title>
      <p id="d1e926">The MLS instrument flies onboard the Aura satellite in a polar orbit with a
continuous record that begins in July 2004. The Aura spacecraft has an
equatorial crossing time of 13:45 (local solar equatorial crossing time of 13:45) (ascending node) with
approximately 15 orbits per day on average. The MLS measures thermal
emissions at the atmospheric limb and provides vertical profiles of several
atmospheric constituents <xref ref-type="bibr" rid="bib1.bibx80" id="paren.47"/>. MLS allows the retrieval of
about 3500 profiles per day with a nearly global spatial coverage between
82<inline-formula><mml:math id="M61" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and 82<inline-formula><mml:math id="M62" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N. Each profile is spaced by about 165 km
along the orbit track. The recommended useful pressure range
<xref ref-type="bibr" rid="bib1.bibx43" id="paren.48"/> for the MLS measurements of the versions v3 and v4 is
from 261 to 0.02 hPa, with a vertical resolution between 2.5 and 6 km,
depending on altitude.</p>
      <p id="d1e953">For this study we used version 4.2 of the MLS ozone product
<xref ref-type="bibr" rid="bib1.bibx65" id="paren.49"/>. Notable improvements of the v4.2, compared to the
earlier versions v3.3 and v3.4, show a reduction in the severity and frequency of
cloud impacts on ozone determination. For more information, users of MLS Aura
L2 v4.2 should refer to the EOS MLS Level 2 Version 4 Quality Document by
<xref ref-type="bibr" rid="bib1.bibx44" id="text.50"/>. MLS ozone profiles show good quality in the UTLS, with a
precision of about 5 %. Biases for MLS ozone profiles are about 2 % in
the stratosphere but they increase in the upper troposphere and can be as
high as 20 % at the 215 hPa level <xref ref-type="bibr" rid="bib1.bibx29" id="paren.51"/>. To avoid the
introduction of biases at this level in our analyses we have taken the MLS
ozone data only between 12.12 and 177.83 hPa.</p>
</sec>
</sec>
<sec id="Ch1.S2.SS2">
  <title>Validation measurements</title>
<sec id="Ch1.S2.SS2.SSS1">
  <title>The OMI-MLS residual method and the Ozone ENSO Index</title>
      <p id="d1e977">The OMI instrument, is one among a total of four instruments onboard the Aura
satellite. It is a nadir-viewing imaging spectrometer that measures the solar
radiation reflected by Earth's atmosphere and surface <xref ref-type="bibr" rid="bib1.bibx39" id="paren.52"/>. It
makes spectral measurements in the ultraviolet (270–314 and 306–380 nm)
and visible 350–500 nm wavelength regions at 0.5 nm resolution. OMI
provides measurements with a daily global coverage and a very high horizontal
spatial resolution of 13 km <inline-formula><mml:math id="M63" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 24 km at nadir <xref ref-type="bibr" rid="bib1.bibx20" id="paren.53"/>.
Retrieval errors of the OMI data vary from 6 to 35 % in the troposphere
<xref ref-type="bibr" rid="bib1.bibx42" id="paren.54"/>. Total column ozone from OMI have been derived using the TOMS
version 8 algorithm <xref ref-type="bibr" rid="bib1.bibx90" id="paren.55"/>.</p>
      <p id="d1e999">To derive TCO with the OMI-MLS residual method, <xref ref-type="bibr" rid="bib1.bibx90" id="text.56"/> subtracted
the stratospheric ozone columns retrieved with MLS from the OMI total column.
They selected OMI pixels with near clear-sky conditions (radiative cloud
fraction <inline-formula><mml:math id="M64" display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 30 %). Stratospheric MLS data were spatially interpolated
each day on a coarser regular grid. The tropopause height used for the TCO
cutoff between OMI and MLS comes from the National Centers for Environmental
Prediction (NCEP) using the 2 K km<inline-formula><mml:math id="M65" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> lapse rate tropopause definition
<xref ref-type="bibr" rid="bib1.bibx18" id="paren.57"/> of the World Meteorological Organization (WMO). We used
OMI-MLS data from the NASA GODDARD website for tropospheric ozone
(<uri>http://acd-ext.gsfc.nasa.gov/Data_services/</uri>). All available daily data
have been averaged to compute monthly means with a latitude–longitude
resolution of 1<inline-formula><mml:math id="M66" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M67" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1.25<inline-formula><mml:math id="M68" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>.</p>
      <?pagebreak page6943?><p id="d1e1056">There is no single universal ENSO index reproducing oceanic and atmospheric
physical conditions over the tropical Pacific <xref ref-type="bibr" rid="bib1.bibx77" id="paren.58"/>. Many
ENSO indices have been developed using for instance SST and precipitation <xref ref-type="bibr" rid="bib1.bibx77 bib1.bibx19" id="paren.59"/>. The commonly used
NOAA Niño 3.4 index is derived from SST anomalies. Based on 30 years
of satellite measurements to investigate ENSO's impact on tropical
TCO, <xref ref-type="bibr" rid="bib1.bibx91" id="text.60"/> produced a monthly OEI. Stratospheric column ozone in
the tropical Pacific has very small longitudinal variations of only a few
Dobson units. This has been shown in the previous studies from SAGE, UARS
HALOE, UARS MLS and AURA MLS stratospheric O<inline-formula><mml:math id="M69" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> satellite measurements
<xref ref-type="bibr" rid="bib1.bibx89 bib1.bibx91" id="paren.61"/>. Because of this characteristic, the zonal
variation of the TCO in the tropical Pacific is essentially identical to the
east–west variation of total column ozone. Thus TCO alone can be used to
derive the OEI. The OEI is obtained by subtracting the TCO in the region
named Pacific Ocean Center (POC, 15<inline-formula><mml:math id="M70" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–15<inline-formula><mml:math id="M71" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N,
110–180<inline-formula><mml:math id="M72" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W) from the TCO in the region Indonesia with
Indian Ocean (IIO, 15<inline-formula><mml:math id="M73" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–15<inline-formula><mml:math id="M74" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 70–140<inline-formula><mml:math id="M75" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) each
month. To compute the TCO, the altitude of the tropopause must be known.
<xref ref-type="bibr" rid="bib1.bibx91" id="text.62"/> used tropopause heights derived from the NCEP data. The
tropopause is defined as the lowest level, with respect to altitude, at which
the temperature lapse rate decreases to 2 <inline-formula><mml:math id="M76" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>C km<inline-formula><mml:math id="M77" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> or less and
does not exceed 2 K km<inline-formula><mml:math id="M78" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for 2 km above. We adopted this tropopause
computation to derive the OEI from our analyses. Tropopause pressures, used
to compute the Ozone Index with the assimilation of both IASI-MLS and MLS
data only, are comprised between 80 hPa at low latitudes and 500 hPa at high
latitudes.</p>
</sec>
<sec id="Ch1.S2.SS2.SSS2">
  <title>Ozonesondes</title>
      <p id="d1e1178">Ozonesondes are launched in many locations over the world on a weekly basis,
measuring vertical profiles of O<inline-formula><mml:math id="M79" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentration with a high vertical
resolution of 150–200 m, from the ground to approximately 10 hPa. Data are
collected by the World Ozone and Ultraviolet Radiation Data Center (WOUDC,
<uri>http://www.woudc.org</uri>). During the 6 years considered in this study
(2008 to 2013), only 270 ozone soundings are available for the Pacific area
between 15<inline-formula><mml:math id="M80" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–15<inline-formula><mml:math id="M81" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and 70<inline-formula><mml:math id="M82" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E–110<inline-formula><mml:math id="M83" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>). We divide this area into two regions: IIO and POC, which are
represented by the two blue rectangles in Fig. <xref ref-type="fig" rid="Ch1.F2"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><caption><p id="d1e1236">Map of WOUDC ozonesonde localization between
15<inline-formula><mml:math id="M84" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and 15<inline-formula><mml:math id="M85" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N. The red circles mark ozonesonde stations
between 70<inline-formula><mml:math id="M86" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E and 110<inline-formula><mml:math id="M87" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W. Green squares are ozonesonde
stations elsewhere in the tropical band used hereafter. The two blue squares
define the IIO region (15<inline-formula><mml:math id="M88" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–15<inline-formula><mml:math id="M89" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and
70–140<inline-formula><mml:math id="M90" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) and the POC region (15<inline-formula><mml:math id="M91" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–15<inline-formula><mml:math id="M92" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and
180–110<inline-formula><mml:math id="M93" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W) referred to in this study.</p></caption>
            <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018-f02.png"/>

          </fig>

      <p id="d1e1336">WOUDC ozonesonde measurements used for the validation are considered as a
reference. Despite their sparse geographical distribution, several studies
have used the WOUDC database to validate global models and satellite retrievals
<xref ref-type="bibr" rid="bib1.bibx30 bib1.bibx48 bib1.bibx24" id="paren.63"/>.</p><?xmltex \hack{\newpage}?>
</sec>
</sec>
<sec id="Ch1.S2.SS3">
  <title>Analyses</title>
<sec id="Ch1.S2.SS3.SSS1">
  <title>Chemical transport model</title>
      <p id="d1e1355">MOCAGE is a three-dimensional CTM based on a semi-Lagrangian advection
scheme <xref ref-type="bibr" rid="bib1.bibx86" id="paren.64"/> developed for both tropospheric and
stratospheric applications. Multiple nested domains with different horizontal
resolutions can be used within MOCAGE, as well as chemical and physical
parameterizations of increasing complexity. The different configurations of
MOCAGE have been validated against in situ, satellite and ground-based
measurements in several studies
<xref ref-type="bibr" rid="bib1.bibx35 bib1.bibx73 bib1.bibx10 bib1.bibx33 bib1.bibx66" id="paren.65"/>. For this
study, a global horizontal resolution of 2<inline-formula><mml:math id="M94" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M95" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 2<inline-formula><mml:math id="M96" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> has
been used with 60 sigma hybrid vertical levels from the surface up to
0.1 hPa. The vertical resolution goes from about 40 m in the boundary
layer, to about 500 m in the free troposphere and to approximately 800 m in
the upper troposphere and lower stratosphere. The model uses winds,
temperature and ground pressure from the European Center for Medium-Range
Weather Forecasts (ECMWF) ERA-Interim reanalysis <xref ref-type="bibr" rid="bib1.bibx9" id="paren.66"/>.</p>
      <?pagebreak page6944?><p id="d1e1393">For the chemical scheme we use the simplified ozone chemistry scheme
developed by <xref ref-type="bibr" rid="bib1.bibx11" id="text.67"/>, based on the linearization of the
destruction and production rates of ozone. <xref ref-type="bibr" rid="bib1.bibx27" id="text.68"/> have shown that
with this simplified chemical scheme it is possible to obtain O<inline-formula><mml:math id="M97" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> analyses
from IASI data of comparable quality to those obtained using more complex
chemical schemes. The use of this simplified scheme reduces numerical costs,
which is highly beneficial for the production of long chemical reanalyses
such as the ones discussed in this study. Since the linearized chemistry
scheme does not have any longitudinal variation, the longitudinal ozone
variability that is reproduced by the model (e.g., in correspondence of the
Walker circulation, see Sect. <xref ref-type="sec" rid="Ch1.S3.SS2.SSS1"/>) results only from the ozone
transport.</p>
</sec>
<sec id="Ch1.S2.SS3.SSS2">
  <title>Assimilation algorithm</title>
      <p id="d1e1419">The chemical data assimilation system for MOCAGE is developed at CERFACS and
has already been used for several applications at both regional and global
scales <xref ref-type="bibr" rid="bib1.bibx26 bib1.bibx67" id="paren.69"/>. The MOCAGE assimilation system was part
of the first international exercise of satellite ozone assimilation
<xref ref-type="bibr" rid="bib1.bibx30" id="paren.70"/> and it currently provides operational air quality analyses
for the european project CAMS <xref ref-type="bibr" rid="bib1.bibx47" id="paren.71"/>. The assimilation
configuration used for this study is based on the 4D-Var algorithm in a
“perfect model” framework. Compared to the 3D-Var algorithm, the 4D-Var
allows a better exploitation of satellite observations with large spatial and
temporal fingerprint <xref ref-type="bibr" rid="bib1.bibx49" id="paren.72"/>. The cost function is minimized
using the limited-memory BFGS (Broyden–Fletcher–Goldfarb–Shanno) method
<xref ref-type="bibr" rid="bib1.bibx40" id="paren.73"/> and the three-dimensional background error covariance matrix
(<bold>B</bold>) is modeled through a diffusion equation <xref ref-type="bibr" rid="bib1.bibx81" id="paren.74"/>.</p>
      <p id="d1e1444">The IASI partial O<inline-formula><mml:math id="M98" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> columns (1000–345 hPa) and MLS profiles have been
assimilated in the troposphere and in the stratosphere respectively to
constrain the ozone concentration along the full atmospheric column. For this
study, the choice of the assimilated column top (345 hPa) has been taken
based on SOFRID averaging kernels found over the tropics <xref ref-type="bibr" rid="bib1.bibx6" id="paren.75"/>.
The objective was to minimize the extent of the atmospheric layer where both
MLS and IASI can have a direct impact. This avoids to some extent the need to
quantify and account for possible biases between the two instruments.
Before the assimilation, IASI data have been averaged to obtain 2<inline-formula><mml:math id="M99" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> by
2<inline-formula><mml:math id="M100" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> pixels to match the model resolution. The smoothing equation based
on the averaging kernels (AKs) and on the a priori profile in the troposphere
has been applied to the profiles from the model to account for the limited
sensitivity of IASI retrievals in the troposphere (see
<xref ref-type="bibr" rid="bib1.bibx7" id="author.76"/>, <xref ref-type="bibr" rid="bib1.bibx7" id="year.77"/>). The description of the
linear retrieval equation can be found in <xref ref-type="bibr" rid="bib1.bibx6" id="text.78"/>.
<xref ref-type="bibr" rid="bib1.bibx27" id="text.79"/> found global biases of 10 % in the troposphere-assimilating IASI-SOFRID product in MOCAGE. When they removed 10 % of the
values in the IASI observations, the biases in the analyses were
significantly reduced. The same correction has been applied in this study.</p>
      <p id="d1e1490">Most of the parameters of the assimilation algorithm used to compute the
reanalyses in this study are based on the study of <xref ref-type="bibr" rid="bib1.bibx27" id="text.80"/>. The
validation of a short reanalysis of 2 months against ozonesondes (not
shown) has been used to further optimize some of these parameters. The
background and observation errors are defined as follows. <xref ref-type="bibr" rid="bib1.bibx27" id="text.81"/>
have assimilated IASI and MLS data globally with a background error standard
deviation equal to 30 % of the modeled ozone profile in the troposphere and
5 % in the stratosphere. Based on local validation in the tropics, we found
slightly superior results using an error standard deviation of 15 instead
of 30 % in the troposphere. Therefore, this choice has been taken for the
6-year reanalyses. We specify the background error variances as a percentage
of the modeled ozone profile equal to 15 % in the troposphere and 5 % in
the stratosphere. These values were established through a global validation
of ozone forecasts against ozonesondes. We use horizontal correlation length
that differs for meridional and zonal dimensions. The meridional length scale
is fixed to a constant value of 300 km and the zonal length scale varies
from 500 km at the equator to 100 km at the poles. Further tests led us to
deactivate the vertical error correlation, compared to the value of one grid
point used in the previous study <xref ref-type="bibr" rid="bib1.bibx27" id="paren.82"/>. Ozonesonde validation
has shown a 20 % decrease in bias close to the tropopause when deactivating
the vertical correlation, the scores remaining the same elsewhere. The reason
for such improvement is due to the relatively coarse vertical resolution of
the model compared to the magnitude of the ozone gradient at the tropopause.
When a nonzero error correlation is used, large assimilation increments due
to the lowermost MLS observations can spread into the upper troposphere and
degrade the ozone concentration. For IASI data we set the variance of the
observation error equal to 15 % of the measured ozone columns. The error
covariance matrix of the MLS retrieval is prescribed from retrieval product
of MLS measurements.</p>
</sec>
</sec>
</sec>
<sec id="Ch1.S3">
  <title>Results</title>
      <p id="d1e1510">We have performed three ozone simulations covering the period 2008 to 2013.
The first simulation, called Direct Model (DM), has been produced by running the
MOCAGE CTM without data assimilation. The model is initialized with a
climatology on 1 November 2007 to allow for a spin-up period of 2 months.
The second simulation, named MLS-a, started in January 2008 with the
assimilation of MLS profiles for the whole period. Finally, the third
simulation (IASI-a) was produced with the assimilation of IASI tropospheric
O<inline-formula><mml:math id="M101" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> columns and MLS stratospheric O<inline-formula><mml:math id="M102" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> profiles. Both MLS-a and IASI-a are
initialized with the direct model output on 1 January 2008. For the three
simulations the outputs are recorded every 6 hours.</p>
      <?pagebreak page6945?><p id="d1e1531">The main results are outlined as follows. Section <xref ref-type="sec" rid="Ch1.S3.SS1"/>
contains the validation of the simulations against ozonesondes. The first
validation (Sect. <xref ref-type="sec" rid="Ch1.S3.SS1.SSS1"/>) has been done considering all the
measurements available in the latitude band between
15<inline-formula><mml:math id="M103" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and 15<inline-formula><mml:math id="M104" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, providing a statistically significant
validation in the tropical region. The following section (Sect. <xref ref-type="sec" rid="Ch1.S3.SS1.SSS2"/>)
limits the comparison with O<inline-formula><mml:math id="M105" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> soundings over the region directly
influenced by ENSO events. In Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/> we analyze the temporal and
spatial variability of TCO during the period 2008–2013. The link between sea
surface temperature and ozone variability is studied with the OMI-MLS
estimations (see Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>). The objective is to evaluate how modeled
ozone distributions reproduce the observed ozone variability over the Pacific
ocean during the normal conditions of the Walker cell and during ENSO events.
In Sect. <xref ref-type="sec" rid="Ch1.S3.SS2.SSS2"/>, we compare the Ozone ENSO Index (OEI), computed using the
previous datasets, to the Niño 3.4 index, to demonstrate the added value
of IASI tropospheric assimilation for long-term ozone monitoring. Finally, in
Sect. <xref ref-type="sec" rid="Ch1.S3.SS2.SSS3"/> the vertical distributions of ozone are examined over two
regions (eastern Asia and Indonesia and over the Pacific Ocean) to highlight
the footprint of ENSO within the three model simulations.</p>
<sec id="Ch1.S3.SS1">
  <title>Validation with ozonesonde measurements</title>
<sec id="Ch1.S3.SS1.SSS1">
  <title>The equatorial latitudes</title>
      <p id="d1e1586">The O<inline-formula><mml:math id="M106" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> data have been treated as follows: (i) the modeled fields have
been collocated with the soundings in space and time, and (ii) the obtained
values have been averaged on a 2-month basis, in order to take into account
a larger number of soundings for statistical evaluations. The collocation was
done with a linear interpolation along each dimension, which results in a
linear interpolation in time of the model's 6-hourly outputs and trilinear
interpolation in space (on both the horizontal and vertical dimensions).</p>
      <p id="d1e1598">Figure <xref ref-type="fig" rid="Ch1.F3"/> shows the comparison between the partial ozone column of
the three simulations and the ozonesonde data in the tropical band
(15<inline-formula><mml:math id="M107" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–15<inline-formula><mml:math id="M108" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N). Partial ozone columns (in DU) and relative
differences (in %) are plotted separately for the TCO (1000–100 hPa),
the boundary layer (1000–750 hPa) and the free troposphere (750–100 hPa).
The TCO from ozonesondes (Fig. <xref ref-type="fig" rid="Ch1.F3"/>a) has maxima in summer–fall and
minima in winter. The observed seasonal variation is a consequence of biomass
burning, which provides precursors for ozone formation in summer–fall. The
emission of gases by biomass burning, such as carbon monoxide and
carbonaceous aerosols, intensifies during the dry season (June–July and
August–October) over both the South American and South African regions
<xref ref-type="bibr" rid="bib1.bibx1 bib1.bibx68" id="paren.83"/>. The ozone columns produced by the DM and MLS-a
simulations do not show the variability measured by the ozonesondes; their
correlation coefficients with the sondes data are lower than 0.76
(Fig. <xref ref-type="fig" rid="Ch1.F3"/>a, b). The IASI-a variability matches the ozonesondes better
with a correlation coefficient of 0.88. In particular the IASI-a simulation
exhibits a year-to-year variability that agrees very well with the ozonesonde
data. This is confirmed by the RSD of
the differences between simulated and observed values: the RSD of IASI-a is
6 % whereas it is about 10 % for MLS-a and MD. The relative differences
between simulated and observed values are presented in Fig. <xref ref-type="fig" rid="Ch1.F3"/>b.
IASI-a is less biased (6 %) than DM and MLS-a, and MLS-a has lower biases
(24 %) than DM (32 %). Biases are lower with MLS-a, compared to DM, due
to the assimilation of MLS stratospheric data. The MLS-a improvement is due
to the direct influence of the lowest assimilated level of MLS (170 hPa)
which brings information on the O<inline-formula><mml:math id="M109" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> distribution in the UTLS region.
Compared to IASI-a the lower accuracy of DM comes from the use of the
simplified ozone scheme, which does not account for the production of
tropospheric ozone by biomass burning.</p>
      <p id="d1e1640">Figure <xref ref-type="fig" rid="Ch1.F3"/>c and d show that the IASI-a tropospheric columns are biased
high in the lower troposphere. In this region, the RSDs of the three
simulations are very similar, implying a similar variability compared to
ozonesondes, even if IASI-a matches the ozonesondes slightly better. However,
IASI-a is half as accurate for the boundary layer O<inline-formula><mml:math id="M110" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> column than for the
TCO and its biases are higher than MD and MLS-a. Larger biases in the
boundary layer are a consequence of both the low degrees of freedom
of IASI retrievals in the troposphere and the presence of a DM
bias with opposite sign between the free troposphere and the boundary layer.
The positive correction provided by IASI assimilation in the free troposphere
propagates downward in the boundary layer, therefore increasing the original
DM bias.</p>
      <p id="d1e1654">Ozone concentration and biases of the IASI-a simulation in the free
troposphere (Fig. <xref ref-type="fig" rid="Ch1.F3"/>e and Fig. <xref ref-type="fig" rid="Ch1.F3"/>f) show much better results
than the two other simulations. As can be seen, the sensitivity of the
IASI measurements is larger in the mid- and upper troposphere. The RSD of
IASI-a is around 6 % instead of 11 % for DM and 9 % for MLS-a in the
middle–upper troposphere (Fig. <xref ref-type="fig" rid="Ch1.F3"/>f). The added value of IASI data in
the middle troposphere is particularly remarkable in the case of bias, which
is 2 % for IASI-a instead of 41 and 32 % for DM and MLS-a, respectively.
Since the boundary layer (1000–750 hPa) corresponds approximately to 12 %
of the TCO (1000–100 hPa), the overestimation of the ozone column by IASI-a
does not have a major impact on the TCO used for our study of the ENSO-O<inline-formula><mml:math id="M111" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
correlation, which is the main objective of this study.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><caption><p id="d1e1675">Time series of partial ozone columns (<bold>a</bold>,
<bold>c</bold>, <bold>e</bold>, in DU) from the IASI-a (red curves), the MLS-a (blue
curve), and the DM (green curve) plotted versus several stations measurements
from WOUDC (black curves). Data are 2-month averages over the area
15<inline-formula><mml:math id="M112" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–15<inline-formula><mml:math id="M113" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and 180<inline-formula><mml:math id="M114" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W–180<inline-formula><mml:math id="M115" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E for
<bold>(a)</bold>, the ozone column between 1015 and 100 hPa <bold>(b)</bold>, the boundary layer (1015–750 hPa) <bold>(c)</bold>,
<bold>(d)</bold> and the
free troposphere (750–100 hPa) <bold>(e)</bold>, <bold>(f)</bold>. Biases in percentages are shown in
<bold>(a)</bold>, <bold>(c)</bold> and <bold>(e)</bold>. Mean biases, correlation coefficients
and standard deviations are also given (between brackets in <bold>b</bold>,
<bold>d</bold> and <bold>f</bold>).</p></caption>
            <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018-f03.png"/>

          </fig>

</sec>
<sec id="Ch1.S3.SS1.SSS2">
  <title>From eastern Africa to South America: focus on the ENSO</title>
      <p id="d1e1774">To study the ENSO we divide the region of interest (latitude ranges from
15<inline-formula><mml:math id="M116" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S to 15<inline-formula><mml:math id="M117" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and longitude ranges from 70<inline-formula><mml:math id="M118" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E to
110<inline-formula><mml:math id="M119" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W) in two areas (see Fig. <xref ref-type="fig" rid="Ch1.F2"/>): the first one, called
IIO, has a longitude range between 70 and 140<inline-formula><mml:math id="M120" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>E while the
second one, called POC, is located between 180 and 110<inline-formula><mml:math id="M121" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W. Three
ozonesonde stations are available for both regions, two in the IIO region and
one in the POC region (Table <xref ref-type="table" rid="Ch1.T1"/>).</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><caption><p id="d1e1839">Ozonesonde stations at tropical latitudes between
70<inline-formula><mml:math id="M122" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E and 110<inline-formula><mml:math id="M123" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="4">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Name</oasis:entry>  
         <oasis:entry colname="col2">Ozonesondes</oasis:entry>  
         <oasis:entry colname="col3">Localization</oasis:entry>  
         <oasis:entry colname="col4">Coordinates</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">Malaysia</oasis:entry>  
         <oasis:entry colname="col2">443 ECC</oasis:entry>  
         <oasis:entry colname="col3">Kuala Lumpur international airport, Malaysia</oasis:entry>  
         <oasis:entry colname="col4">3<inline-formula><mml:math id="M124" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–101<inline-formula><mml:math id="M125" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Indonesia</oasis:entry>  
         <oasis:entry colname="col2">437 ECC</oasis:entry>  
         <oasis:entry colname="col3">Watukosek, Java Timur, Indonesia</oasis:entry>  
         <oasis:entry colname="col4">8<inline-formula><mml:math id="M126" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–113<inline-formula><mml:math id="M127" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Samoa</oasis:entry>  
         <oasis:entry colname="col2">191 ECC</oasis:entry>  
         <oasis:entry colname="col3">Apia, Samoa</oasis:entry>  
         <oasis:entry colname="col4">13<inline-formula><mml:math id="M128" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–172<inline-formula><mml:math id="M129" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d1e1994">Ozone measurements for each site are available over different time periods.
The Malaysia site provides measurements only between January 2008 and
December 2009, the Indonesia site from January 2008 to December 2012, and the
Samoa site from January 2008 to December 2013. Due to the small number of
ozonesonde measurements, results of the statistical validation presented
here should be considered with more caution than in the previous section. The
main objective of this section is to check whether the reanalysis can capture
strong local variations of TCO due to ENSO.</p>
      <p id="d1e1997">Figure <xref ref-type="fig" rid="Ch1.F4"/> shows the statistics of the IASI-a O<inline-formula><mml:math id="M130" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> simulation versus
the three records from the ozone soundings. Time series are computed in the
same manner as the time series over the tropical band discussed in the
previous section (Sect. <xref ref-type="sec" rid="Ch1.S3.SS1.SSS1"/>). From January 2008 to December
2009, TCOs from the ozonesondes located in the IIO region (Fig. <xref ref-type="fig" rid="Ch1.F4"/>a,
c) and those located in the POC region (Fig. <xref ref-type="fig" rid="Ch1.F4"/>e), has a seasonal
variability, with maxima in boreal summer and minima in boreal winter. This
ozone seasonality is caused by the biomass combustion over the western
Pacific Ocean near New Guinea during the dry period <xref ref-type="bibr" rid="bib1.bibx36" id="paren.84"/>. Among
the countries of southern Asia, Indonesia is known as the country with the
third-highest biomass burning emissions
<xref ref-type="bibr" rid="bib1.bibx71" id="paren.85"/>. During the year 2010 and over the IIO region
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>c), the variability of ozone concentrations has a different
seasonality. We see a peak of ozone during March 2010 over Indonesia (26 DU)
whereas there is a minimum in Samoa (12 DU) (Fig. <xref ref-type="fig" rid="Ch1.F4"/>e). This ozone
rise over the IIO region is linked with subsidence, generated by the El
Niño event starting in January 2010 (see Fig. <xref ref-type="fig" rid="Ch1.F1"/>). El Niño
intensifies the subsidence and therefore dry conditions and biomass burning
over southern Asia <xref ref-type="bibr" rid="bib1.bibx50 bib1.bibx13" id="paren.86"/>. From September 2010 to
August 2011, the TCO values decrease to an average of about<?pagebreak page6947?> 20 DU over
Indonesia. This decrease in tropospheric ozone is due to the other phase of
ENSO: La Niña. As we have already mentioned (Fig. <xref ref-type="fig" rid="Ch1.F1"/>), La
Niña strengthens the convection over the IIO causing a minimum in the
TCO. Hence, there is a lower TCO over Indonesia (around 20 DU) than over
Samoa (around 28 DU). After summer 2011 the ENSO disappears and the TCO
returns to normal seasonality.</p>
      <p id="d1e2037">IASI-a reproduces quite well the variability measured by the ozonesondes
during normal conditions of the Walker circulation (2008–2009) and during
the ENSO (2010–2011). In particular, IASI-a agreement with the ozonesondes
is better over the POC region (Samoa), where the correlation coefficient is
0.96, than over Indonesia and Malaysia where the coefficients are around 0.7.
However, the relative difference between IASI-a and the ozonesondes is larger
over the POC region (Fig. <xref ref-type="fig" rid="Ch1.F4"/>f) than over the IIO region
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>b, d), with an overestimation of the ozone columns by about
17 % in Samoa. Mean biases are around 3–5 % for over Indonesia and
Malaysia, showing that IASI-a reproduces quite well the ozone variability
during normal conditions of the Walker circulation. Equally, IASI-a reproduces
the maximum over Indonesia and the minimum over Samoa during the 2010 El
Niño event, as well as the TCO minima generated during La Niña over
the IIO region. As already discussed, biases observed in the POC and IIO
regions come from the decreased sensitivity of IASI in the boundary layer,
and from the lack of adequate representation of the chemistry in the lower
troposphere by the linear scheme used within MOCAGE. The three simulations
(IASI-a, MD and MLS-a) have identical biases in the boundary layer compared
to the ozone soundings (figures not shown). Biases in the boundary layer are
higher in the POC region (around 45 %) compared to the IIO region (around
20 %). However, in the POC region, the variability of the three simulations
are remarkably well correlated with the ozonesondes, with coefficient
correlations higher than 0.85 (not shown).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><caption><p id="d1e2046">Comparisons between IASI-a (in red) and ozonesondes (in
black). Time series of the TCO (in DU) are plotted on the left and relative
differences are on the right for the sites of <bold>(a, b)</bold> Malaysia,
<bold>(c, d)</bold> Indonesia and <bold>(e)</bold>, <bold>(f)</bold> Samoa.</p></caption>
            <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018-f04.png"/>

          </fig>

      <p id="d1e2067">To summarize, the IASI-a simulation reproduces well the O<inline-formula><mml:math id="M131" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> variability
observed with the ozonesondes for the tropical latitudes and for both regions
of POC and IIO. The seasonal oscillations of ozone, caused by the
anthropogenic pollution and by ENSO, are reproduced by IASI-a despite a
slight overestimation of about 4 % in the IIO region and around 17 % in
the POC region. The IASI-a simulation is thus adequate to study ozone
variability during ENSO events since biases are not very large over the
period under study.</p>
</sec>
</sec>
<sec id="Ch1.S3.SS2">
  <title>Temporal and spatial variability of ozone during ENSO</title>
<sec id="Ch1.S3.SS2.SSS1">
  <title>Characterization of ENSO and footprints on SST and tropospheric ozone content</title>
      <p id="d1e2091">In this section we consider the link between SST
and tropospheric ozone during ENSO events. Previous studies have highlighted
the link between SST anomalies and ENSO dynamics
<xref ref-type="bibr" rid="bib1.bibx57 bib1.bibx3 bib1.bibx79" id="paren.87"/>. Colder SST in the POC region is
associated with La Niña whereas El Niño has warmer SST than under normal
conditions <xref ref-type="bibr" rid="bib1.bibx77" id="paren.88"/>. Variations in TCO concentrations are a
combination of biomass burning rejecting large quantities of ozone precursors
<xref ref-type="bibr" rid="bib1.bibx13" id="paren.89"/> and an eastward shift in the tropical convection of the
Walker circulation associated with SST changes <xref ref-type="bibr" rid="bib1.bibx12 bib1.bibx72" id="paren.90"/>.
The correlation between SST and TCO have already been characterized using
OMI-MLS data; our objective is to see if similar correlations can be derived
using the model simulations. To this end, we have taken SST data from the
Giovanni Interactive Visualization and Analysis GES DISC: Goddard Earth
Sciences, data and Information Services Centre
(<uri>https://disc.gsfc.nasa.gov</uri>). The SST data were measured by the
instrument MODIS (Moderate Resolution Imaging Spectroradiometer) aboard the
Aqua satellites (NASA Earth Observing System platforms).</p>
      <p id="d1e2109">Figure <xref ref-type="fig" rid="Ch1.F5"/> shows the time versus longitude Hovmöller diagram,
averaged between 15<inline-formula><mml:math id="M132" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and 15<inline-formula><mml:math id="M133" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, of the monthly mean SST
and the OMI-MLS measurements. SST over the Pacific ocean has a characteristic
geographic distribution (Fig. <xref ref-type="fig" rid="Ch1.F5"/>a), with the warmest water in the IIO
region (70–140<inline-formula><mml:math id="M134" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) and coldest water in the POC region
(180–110<inline-formula><mml:math id="M135" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W). The link between SST and TCO <xref ref-type="bibr" rid="bib1.bibx12 bib1.bibx14" id="paren.91"/> is observed comparing the SST (Fig. <xref ref-type="fig" rid="Ch1.F5"/>a) with OMI-MLS
measurements (Fig. <xref ref-type="fig" rid="Ch1.F5"/>b). The warmest water-induced convective
movements result in a TCO decrease and vice versa for the coldest water. During El Niño (January 2010) the warm SST shifts from
the IIO region to the POC region. These eastward shifts in SST coincide with
eastward shifts of TCO from July 2008 to January 2010. During La Niña
(occurred between September 2010 and January 2011) an opposite condition
occurs with the strengthening of colder SST between 80 and 150<inline-formula><mml:math id="M136" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W.
In this region of colder SST (Fig. <xref ref-type="fig" rid="Ch1.F5"/>a), higher TCO (26–32 DU) is
located between the coast of South America and 140<inline-formula><mml:math id="M137" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>b). The eastward shift of SST occurring from January 2011 to
December 2013 corresponds to the return of normal conditions over the Pacific
ocean and impacts TCO with an eastward shift.</p>
      <p id="d1e2183">To compare the three model simulations, with OMI-MLS, we have computed
anomalies of tropospheric ozone of each dataset for the period 2008–2013
(Fig. <xref ref-type="fig" rid="Ch1.F6"/>). The anomalies are calculated by subtracting the
time-averaged TCO to each TCO determination and this difference has been
divided by the mean TCO. The TCO anomalies are expressed in percentage. The
variability of TCO, observed previously with OMI-MLS measurements in
Fig. <xref ref-type="fig" rid="Ch1.F5"/>, is also clearly visible with the TCO anomaly
(Fig. <xref ref-type="fig" rid="Ch1.F6"/>a). The TCO with values 20 % lower than average are
located in the IIO region. The TCO with values 20 % higher than average are
located close to South American coasts. The El Niño event on January 2010
has a significant impact on TCO, with 20 % higher values in the IIO
region and 10 % lower in the POC region. The La Niña event that follows
shows different localization on the TCO maximum with a maximum between 110
and 80<inline-formula><mml:math id="M138" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W.<?pagebreak page6948?> Part of the TCO variability in the eastern and western
Pacific Ocean linked with the Walker circulation is reproduced with the DM
simulation (Fig. <xref ref-type="fig" rid="Ch1.F6"/>b). The TCO with values 10 % higher (10 %
lower) than average are located in POC (IIO) region. However, the amplitude
of the TCO anomalies from the DM simulation is much lower compared to
OMI-MLS. Since the chemical scheme used in the MOCAGE model has no
longitudinal forcing in the chemical tendencies, the TCO anomalies in the DM
simulation are only due to changes in the equatorial circulation and the
associated ozone transport. The ECMWF analyses capture the dynamics
associated with the Walker circulation and to ENSO and hence drive the
variations of the TCO seen in the DM simulation. The assimilation of MLS
O<inline-formula><mml:math id="M139" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> profiles in the stratosphere does not change the structures and
percentages of anomalies of the TCO much, and the results of the MLS-a
simulation (Fig. <xref ref-type="fig" rid="Ch1.F6"/>c) are similar to those of the DM. The eastward
shift during El Niño and higher TCO in the POC region during La Niña
are represented with both simulations but the TCO anomalies for both
simulations are 10 % lower than with those of OMI-MLS. Basically the ENSO
impacts the troposphere and little information is brought by the assimilation
of MLS data. The eastward shift during El Niño and higher TCO
in the POC region during La Niña are underestimated by both simulations.
Compared to DM and MLS-a the TCO variability is much better reproduced with
IASI-a (Fig. <xref ref-type="fig" rid="Ch1.F6"/>d). The amplitude of the TCO changes caused by El
Niño and La Niña compares very well with the OMI-MLS observations.
However, small differences appear between IASI-a and OMI-MLS. Over the IIO
region during El Niño the TCO anomaly is 10 % lower with IASI-a than
with OMI-MLS. In addition, the location of the TCO maximum during La Niña
is located in the whole POC region with IASI-a and in the eastern part of the
POC region with OMI-MLS.</p>
      <p id="d1e2217">Overall, the anomalies of the TCO reproduced by IASI-a are in good agreement
with those of OMI-MLS. The improvement compared to the DM and MLS-a
simulations is very significant, thus demonstrating the usefulness of the
IASI data for the ozone evaluation in the troposphere. Equally, the
assimilation process is efficient to follow ozone variability and the
resulting IASI-a analysis appears to give a consistent dataset for the study
of the ozone variability. The advantage of IASI-a over OMI-MLS is that the
analyses are<?pagebreak page6949?> fully four-dimensional with 6-hourly outputs and resolved information on
the vertical dimension. The vertical distributions are studied in
Sect. <xref ref-type="sec" rid="Ch1.S3.SS2.SSS3"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><caption><p id="d1e2225"><bold>(a)</bold> Time versus longitude Hovmöller diagram
of the SST (in <inline-formula><mml:math id="M140" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>C). <bold>(b)</bold> Same diagram from the OMI-MLS
data. The data are monthly means from January 2008 to December 2013 and
area-averaged between latitudes 15<inline-formula><mml:math id="M141" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and 15<inline-formula><mml:math id="M142" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N. Also
included on the bottom are the corresponding maps of the Hovmöller diagram.</p></caption>
            <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018-f05.png"/>

          </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><caption><p id="d1e2268">Longitude Hovmöller diagrams of TCO anomalies for
<bold>(a)</bold> OMI-MLS measurements, <bold>(b)</bold> Direct Model,
<bold>(c)</bold> MLS-a and <bold>(d)</bold> IASI-a between 2008 and 2013. Longitudes
are identical to Fig. <xref ref-type="fig" rid="Ch1.F5"/>: between 40<inline-formula><mml:math id="M143" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E and 80<inline-formula><mml:math id="M144" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W.
Anomalies are expressed in percentage.</p></caption>
            <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018-f06.jpg"/>

          </fig>

</sec>
<sec id="Ch1.S3.SS2.SSS2">
  <title>Intercomparison of Ozone ENSO Indices</title>
      <p id="d1e2316">The OEI is the TCO difference computed between the IIO region
(70–140<inline-formula><mml:math id="M145" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) and the POC region (180–110<inline-formula><mml:math id="M146" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W). The
resulting time series are then deseasonalized. This deseasonalization is done
to remove the signal of the annual cycle <xref ref-type="bibr" rid="bib1.bibx91" id="paren.92"/>. OEI is a strong
indicator of the ENSO intensity influencing the tropospheric ozone over IIO
and POC regions <xref ref-type="bibr" rid="bib1.bibx91" id="paren.93"/>. It is considered as a basic diagnostic
tool to evaluate the ability of the models to reproduce changes in
tropospheric ozone linked with ENSO <xref ref-type="bibr" rid="bib1.bibx91 bib1.bibx92" id="paren.94"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><caption><p id="d1e2348"><bold>(a)</bold> Monthly mean tropospheric Ozone ENSO Index
(in DU) derived from the OMI-MLS data (grey line). Also shown is the
Niño 3.4 monthly temperature anomaly ENSO index (cyan curve, multiplied
by a factor of 3, in Kelvin) and the OEI-Z index derived from the OMI-MLS data
with a deseasonalization followed by a sliding average of 3 months (orange
curve). <bold>(b)</bold> The OMI-MLS data (grey curve) as in the above plot, the
MLS-a (in blue curve), the DM in green curve and the IASI-a (in red curve).
All ENSO indices extend from January 2008 through December 2013.</p></caption>
            <?xmltex \igopts{width=312.980315pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018-f07.png"/>

          </fig>

      <p id="d1e2362">Figure <xref ref-type="fig" rid="Ch1.F7"/> shows the OEI during the period January 2008 to December
2013 computed from our model analyses and from the OMI-MLS data. The OEI
variations are related to ENSO, with maxima during El Niño and minima
during La Niña events. In Fig. <xref ref-type="fig" rid="Ch1.F7"/>a we have plotted the OEI
computed for the OMI-MLS measurements (noted OMI-MLS) and the Niño 3.4
index. The monthly Niño 3.4 is calculated from SST anomalies in the
Pacific Ocean. The Niño 3.4 index calculated from SST is available from
the NOAA website (<uri>http://www.cpc.ncep.noaa.gov/data/indices/</uri>). Sea
surface temperature anomalies were calculated using the monthly Extended
Reconstructed Sea Surface Temperature version 4 (ERSST.v4, 1950–2016 base
period). Also included is the OEI of OMI-MLS smoothed using a 3-month running
average, as computed by <xref ref-type="bibr" rid="bib1.bibx91 bib1.bibx92" id="text.95"/> and called OEI-Z
hereafter. Figure <xref ref-type="fig" rid="Ch1.F7"/>b shows the OEI computed from IASI-a, MLS-a, DM
and OMI-MLS. Our OEI indices from OMI-MLS, DM, MLS-a and IASI-a are computed
without time averaging, by subtraction of TCO in the POC region from TCO
averaged over the IIO region. As defined by the NOAA, the two ENSO phases
occur when the Niño 3.4 index is higher than 0.5 (corresponding to El
Niño) and lower than <inline-formula><mml:math id="M147" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.5 (corresponding to La Niña) during five
consecutive months. Thus, in the analyzed period an El Niño starts on
July 2008 with a maximum on January 2010, and a La Niña starts on
July 2010 with a maximum on January 2011. The two time series of OEI-Z and
OMI-MLS appear remarkably similar (Fig. <xref ref-type="fig" rid="Ch1.F7"/>a), except around
January 2008. For this period they are out of phase with the Niño 3.4.
The discrepancy is attributed to the phase opposition between the interannual
and intraseasonal variability of the TCO <xref ref-type="bibr" rid="bib1.bibx92" id="paren.96"/> linked with the
intraseasonal Madden–Julian Oscillation (MJO, <xref ref-type="bibr" rid="bib1.bibx45 bib1.bibx46" id="altparen.97"/>).
The MJO increases the differences between OEI-Z and OMI-MLS in 2008.
Detailing the effect of MJO on monthly OEI is beyond the scope of our current
study. As expected, the OEI from OMI-MLS shows a consistent variability with
OEI-Z; in particular the maxima and minima agree and are well correlated to
the Niño 3.4 index. Since the OMI-MLS OEI is obtained from monthly
averages it exhibits shorter term variability than OEI-Z and can be directly
compared to the indices derived from the model simulations.</p>
      <p id="d1e2393">The DM OEI (Fig. <xref ref-type="fig" rid="Ch1.F7"/>b, green curve) is negative during the whole
period, corresponding to a tropospheric column higher over the POC region
than over the IIO region. The DM OEI variations show some features of the
ENSO, with a relative maximum in January 2010 followed by a minimum at the end
of the same year, but the intensity is weak: about 3 times lower than
values observed with OMI-MLS. The MLS-a produces an OEI very similar to DM.
As already discussed, constraining the ozone profile in the stratosphere has
little impact on the quality of the modeled ENSO O<inline-formula><mml:math id="M148" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> signal. With the
IASI-a we can quantify the contribution of IASI data in the computed OEI
(Fig. <xref ref-type="fig" rid="Ch1.F7"/>b, red curve). Compared to DM and MLS-a simulations the
IASI-a analysis produces OEI in better agreement with the ones derived from
OMI-MLS. The OEI variations are in phase with a very good match of periods of
maxima and minima. There is, however, a constant bias of approximately 2.4 DU
between the indices of OMI-MLS and IASI-a. As discussed in Sect. <xref ref-type="sec" rid="Ch1.S3.SS1.SSS2"/>,
IASI-a bias in the lower troposphere is larger in the POC region than in the
IIO region. This difference of biases between POC and IIO regions affects the
determination of the OEI. In addition, during ENSO events we have seen from
the Hovmöller plots in Sect. <xref ref-type="sec" rid="Ch1.S3.SS2.SSS1"/> that during La Niña the TCO
maximum with IASI-a is slightly shifted to the western part of the POC region
compared to the OMI-MLS data. The difference in the location of maxima over
the eastern Pacific between OMI-MLS and IASI-a explains part of the
difference in the OEI absolute values during El Niño and La Niña
events (Fig. <xref ref-type="fig" rid="Ch1.F7"/>).</p>
      <p id="d1e2417">Tropospheric ozone variability during ENSO is therefore very well captured
from the OEI variations computed from IASI-a, despite a constant bias in the
boundary layer. Further insights into the vertical distribution of O<inline-formula><mml:math id="M149" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> over
the POC and IIO regions during ENSO are discussed in the next section.</p>
</sec>
<sec id="Ch1.S3.SS2.SSS3">
  <?xmltex \opttitle{Vertical structure of O${}_{3}$}?><title>Vertical structure of O<inline-formula><mml:math id="M150" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula></title>
      <p id="d1e2444">The evaluations of TCO obtained with the OMI-MLS by subtracting stratospheric
ozone from MLS from the total ozone from OMI cannot give information on the
vertical structure of the O<inline-formula><mml:math id="M151" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> anomalies forced by ENSO. This is clearly an
advantage of model assimilations that can give a complete three-dimensional structure of
the ozone fields with no gaps due to orbitography and clouds. We focus here
on the information brought by the assimilation of IASI and MLS data in
describing the vertical ozone response to ENSO in the POC and IIO regions.
Figure <xref ref-type="fig" rid="Ch1.F8"/> shows monthly mean ozone profiles for IASI-a, MLS-a and DM,
over the 6-year record. The tropopause pressure for the three simulations
is about 100 hPa. Ozone concentration in this layer is around 70 ppbv. Due
to the limitations of the model and the lack of information brought by the
two instruments in the boundary layer, as<?pagebreak page6950?> already discussed, we focus our
analysis in the IIO et POC regions on the free troposphere, between 750 and
100 hPa.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8" specific-use="star"><caption><p id="d1e2460">Monthly mean time series of ozone vertical profiles
(units ppbv) versus pressure for the IIO region <bold>(a, c, e)</bold> and the
POC region <bold>(b, d, f)</bold>. The abscissa goes from January 2008 to
December 2013. Panels <bold>(a, b)</bold> correspond to the Direct Model, <bold>(c, d)</bold>
to the MLS-a and <bold>(e, f)</bold> to the IASI-a simulations. Pressure scale
goes from 1013 to 20 hPa.</p></caption>
            <?xmltex \igopts{width=418.255512pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/6939/2018/acp-18-6939-2018-f08.png"/>

          </fig>

      <p id="d1e2484">The DM (Fig. <xref ref-type="fig" rid="Ch1.F8"/>a, b) and MLS-a (Fig. <xref ref-type="fig" rid="Ch1.F8"/>c, d) produce very
close distributions of the vertical ozone concentration. The MLS-a simulation
shows slightly more ozone in the lower stratosphere and upper troposphere,
but the fluctuations of the concentration have similar amplitudes in both
simulations. Particularly noticeable is the signal during the 2010 El
Niño with low ozone values in the POC region during the first months of
the year linked to increased convection and associated upward motions, and an
opposite behavior in the IIO region with subsidence and increased ozone down
to the middle troposphere. This footprint of ENSO is very well captured with
the IASI-a simulation, especially over the POC region. Over that region the
ozone content is lower than 35 ppbv during El Niño and larger than
50 ppbv during La Niña. The information brought by IASI is very
significant, the amplitude of the ozone change between El Niño and La
Niña periods is 2 to 3 times larger with IASI-a assimilation than it is
with DM and MLS-a simulations. If we refer to OEI indices (Fig. <xref ref-type="fig" rid="Ch1.F7"/>)
some ENSO activity is detected in late 2012–early 2013. Indeed an O<inline-formula><mml:math id="M152" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
minimum in early 2013 followed by a maximum in the middle of the year is
clearly visible in the IASI-a assimilation in the POC region. The amplitude
of the ENSO signal on ozone is lower than for the 2010 event, in agreement
with the lower values of the Niño 3.4 index. Also more clearly visible
with IASI-a are the seasonal variations of the ozone content in the IIO
region that is quite regular outside ENSO periods. In that region the annual
periodicity of ozone is much pronounced in comparison to the more erratic
variations shown in the POC region. The regularity of the ozone fluctuation
is more pronounced in IASI-a assimilation than in DM and MLS-a simulations.
In addition to the influence of atmospheric dynamics, biomass burning and the
associated ozone production could trigger the seasonal fluctuations. Such an
ozone production detected by the<?pagebreak page6951?> IASI instrument (and therefore visible in
IASI-a) cannot be reproduced by the DM and MLS-a simulations due to the
simplified chemical scheme.</p>
      <p id="d1e2503">Overall the combination of the IASI ozone tropospheric retrievals and our
4D-Var algorithm produces a very consistent dataset for the study of the
influence of ENSO on the ozone distribution from the stratosphere to the
middle troposphere. The quality of IASI-a, which also includes the
assimilation of MLS, is good in the stratosphere down to the middle troposphere.
In the boundary layer, below 800 hPa, a comprehensive chemical scheme with
adequate emissions should be used to improve the assimilation since there are
no global observations of the ozone content in this layer over the equatorial
regions.</p>
</sec>
</sec>
</sec>
<?pagebreak page6952?><sec id="Ch1.S4" sec-type="conclusions">
  <title>Summary and conclusion</title>
      <p id="d1e2514">A total of 6 years (from January 2008 to December 2013) of 6-hourly
tropospheric ozone fields have been derived by assimilating IASI and MLS
ozone measurements in the MOCAGE CTM. The assimilation of IASI tropospheric
columns combined with MLS stratospheric profiles was first validated against
ozonesondes in the tropical band (15<inline-formula><mml:math id="M153" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–15<inline-formula><mml:math id="M154" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), providing
a statistically robust validation. In the tropical band and over the whole
period, IASI-a gives results similar to ozonesondes and reproduces the ozone
variability well despite a constant bias. Biases in the analysis come from
the low accuracy of the model in the boundary layer. The ozone linear scheme
in MOCAGE does not take surface emissions into account. In addition, IASI has
a weak sensitivity in the boundary layer and therefore does not provide
additional information on O<inline-formula><mml:math id="M155" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> content in this layer. A
second validation has been done over the Pacific ocean and over southern Asia
(longitude band of 70<inline-formula><mml:math id="M156" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E to 110<inline-formula><mml:math id="M157" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W). During the 2008–2013
period, an ENSO event developed with its two phases: El Niño in
winter 2010 and La Niña in winter 2011. IASI-a has been validated in two
areas: the Indonesia and Indian Ocean and the Pacific Ocean Center regions.
In both regions, biases appear and are larger in the POC region. The weak
sensitivity of IASI sounding in the boundary layer is responsible for these
biases. However, the tropospheric ozone variability related to the Walker
Circulation and to the ENSO event is well reproduced with IASI-a.</p>
      <p id="d1e2562">OMI-MLS tropospheric columns have been used and validated by several past
studies. We have used OMI-MLS ozone data to characterize the links between
SST and tropospheric O<inline-formula><mml:math id="M158" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and to compare with our IASI-a assimilation.
Anomalies of TCO have been computed, allowing a comparison between IASI-a and
the two other simulations (Direct Model and MLS-a) with OMI-MLS. Anomalies of
the Direct Model (MOCAGE without assimilation) are similar to<?pagebreak page6953?> anomalies of
MLS-a (assimilation of MLS stratospheric profiles). The good reproduction of
anomalies in terms of location and timing between eastern and western regions
in both simulations are due to the transport forced by the winds from the
ECMWF meteorological analyses. However, the amplitude of anomalies is lower
than in OMI-MLS data. Assimilation of IASI data corrects this behavior, and
the anomalies of IASI-a appear very similar to the OMI-MLS anomalies. In
particular, the IASI data bring essential information to reproduce the
eastward
shift of TCO caused by El Niño.</p>
      <p id="d1e2574">In order to study the ability of IASI-a to reproduce the ozone variability
caused by El Niño and La Niña phases, we have used the OEI. The OEI
represents an essential diagnostic test for models that should be able to
represent ozone features linked with ENSO changes in tropospheric dynamics.
OEI from IASI-a shows variations similar to those of OMI-MLS with a small
bias corresponding to higher TCO over the POC than over the IIO region.
The Direct Model and MLS-a have the same bias. This bias has been located in the
boundary layer with the comparison with the ozonesondes.</p>
      <?pagebreak page6954?><p id="d1e2577">We have also examined the vertical structures of tropospheric ozone in the
IIO and POC regions, with the three simulations (Direct Model, MLS-a and
IASI-a), in order to show the contribution of IASI tropospheric data in the
assimilation. The IASI-a analysis is consistent with the ozone displacements
in adequation with subsidences and convergences generated by El Niño and
La Niña in both IIO and POC regions. The IASI assimilation gives a very
valuable high-resolution dataset suitable to perform analyses of the O<inline-formula><mml:math id="M159" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
variability in the upper and middle troposphere for short-term and
interannual timescales in the tropical band.</p>
      <p id="d1e2590">Overall, the assimilation of stratospheric MLS and tropospheric IASI data
within MOCAGE gives a good representation of the tropospheric ozone
variability linked with ENSO and the Walker circulation. We have shown the
importance of assimilating tropospheric IASI data to provide vertical
information on tropospheric ozone variability, showing the benefit of IASI
analyses for studies on ENSO dynamics. In addition, since ENSO is one of the
most important interannual fluctuations in climate variability, this study is
part of a climate variability perspective. The assimilation of satellite data
is promising for determining the impact of climate variability on
tropospheric chemistry. There are, however, some limitations in our simulations
that have to be addressed. One of them is the bias found in the boundary layer
over the Pacific Ocean that affects the calculation of the OEI. In this study
we have used a linear ozone parameterization to compute the ozone chemical
tendencies. This approach is suitable for the free troposphere and the
stratosphere but is certainly not adequate for the boundary layers. In the
future we plan to use a more comprehensive chemical scheme that accounts for
the surface emissions.</p>
      <p id="d1e2593">With the use of IASI data we have demonstrated here the value of assimilating
satellite data that document the direct information in the tropospheric ozone
content to compute OEI. This approach is promising because many types of data
can enter in an assimilation process, such as the balloon and aircraft
measurements. Improvements in the tropospheric ozone content evaluations can
be expected from an increase in assimilated data. Times series of IASI
analysis could then be derived and used to study the tropospheric ozone
variability over at least a 30-year period. One advantage of infrared
sounders like IASI for climate studies is their good spectral stability over
time, with respect for example to UV instruments. This is an important
feature when trying to determine potentially small climate signals hidden by
large ozone variability, due for example to ENSO. Finally, using a more
detailed chemistry scheme within future ozone reanalyses would also allow
further insights into chemical feedbacks in the context of a changing climate.</p>
</sec>

      
      </body>
    <back><notes notes-type="dataavailability">

      <p id="d1e2601">IASI L1 data were provided by the Laboratory of Aerology.
EOS MLS L2 version 4 is available at <uri>https://mls.jpl.nasa.gov/data/</uri>.
The OMI-MLS tropospheric ozone as well as the OEI-Z index are available at
<uri>http://acd-ext.gsfc.nasa.gov/Data_services/cloud_slice/</uri>. The Nino3.4
index is available from the NOAA website at
<uri>http://www.cpc.ncep.noaa.gov/data/indices/</uri>.</p>
  </notes><notes notes-type="competinginterests">

      <p id="d1e2616">The authors declare that they have no conflict of
interest.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e2622">We would like to thank Jerry R. Ziemke and the Aura Ozone Monitoring
Instrument (OMI) science team of the NASA Goddard Space Flight Center to the
availability of the OMI-MLS data and the OEI-Z Index. We also thank WOUDC for
providing ozonesonde station data and the NASA Jet Propulsion Laboratory for
the availability of Aura MLS data. We also acknowledge the mission scientists
from the NASA GES DISC, who provided the GIOVANNI SST data used in this
research. In addition, we acknowledge la Région
Midi-Pyrénées for financial support and the CNES (Centre National
d'Études Spatiales) for financial sources on the TOSCA project. Thanks
also to Sean Crowell for proofreading an earlier version of this paper.<?xmltex \hack{\newline\newline}?>
Edited by: Jayanarayanan Kuttippurath <?xmltex \hack{\newline}?>Reviewed by: Catherine
Wespes and one anonymous referee</p></ack><ref-list>
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<abstract-html><p>The Infrared Atmospheric Sounder Instrument (IASI) allows global coverage
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