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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-18-7557-2018</article-id><title-group><article-title>Multiple symptoms of total ozone recovery inside the Antarctic vortex during
austral spring</article-title><alt-title>Multiple symptoms of Antarctic total ozone recovery</alt-title>
      </title-group><?xmltex \runningtitle{Multiple symptoms of Antarctic total ozone recovery}?><?xmltex \runningauthor{A. Pazmi\~{n}o et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Pazmiño</surname><given-names>Andrea</given-names></name>
          <email>andrea.pazmino@latmos.ipsl.fr</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Godin-Beekmann</surname><given-names>Sophie</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-3903-3040</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Hauchecorne</surname><given-names>Alain</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-9888-6994</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Claud</surname><given-names>Chantal</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Khaykin</surname><given-names>Sergey</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-5466-1096</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Goutail</surname><given-names>Florence</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1431-1542</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3 aff4">
          <name><surname>Wolfram</surname><given-names>Elian</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6297-4327</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3 aff4 aff5">
          <name><surname>Salvador</surname><given-names>Jacobo</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Quel</surname><given-names>Eduardo</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-9638-0823</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>LATMOS, UVSQ Univ. Paris Saclay, UPMC Univ. Paris 06, CNRS, Guyancourt, France</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>LMD, CNRS, Ecole Polytechnique, Palaiseau, France</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>CEILAP-UNIDEF (MINDEF-CONICET), UMI-IFAECI-CNRS-3351, Villa Martelli, Argentina</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Universidad Tecnológica Nacional, Facultad Regional Bs. As. (UTN-FRBA), Ciudad Autónoma de Buenos Aires, Argentina</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>Universidad Nacional de la Patagonia Austral, Unidad Académica Río Gallegos (UNPA-UARG), Río Gallegos, Argentina</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Andrea Pazmiño (andrea.pazmino@latmos.ipsl.fr)</corresp></author-notes><pub-date><day>31</day><month>May</month><year>2018</year></pub-date>
      
      <volume>18</volume>
      <issue>10</issue>
      <fpage>7557</fpage><lpage>7572</lpage>
      <history>
        <date date-type="received"><day>9</day><month>December</month><year>2017</year></date>
           <date date-type="rev-request"><day>12</day><month>December</month><year>2017</year></date>
           <date date-type="rev-recd"><day>30</day><month>April</month><year>2018</year></date>
           <date date-type="accepted"><day>7</day><month>May</month><year>2018</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2018 </copyright-statement>
        <copyright-year>2018</copyright-year>
      <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/.html">This article is available from https://acp.copernicus.org/articles/.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/.pdf</self-uri>
      <abstract>
    <p id="d1e181">The long-term evolution of total ozone column inside the Antarctic polar
vortex is investigated over the 1980–2017 period. Trend analyses are
performed using a multilinear regression (MLR) model based on various proxies
for the evaluation of ozone interannual variability (heat flux,
quasi-biennial oscillation, solar flux, Antarctic oscillation and aerosols).
Annual total ozone column measurements corresponding to the mean monthly values inside the
vortex in September and during the period of maximum ozone depletion from
15 September   to 15 October   are used. Total ozone columns from
the Multi-Sensor Reanalysis version 2 (MSR-2) dataset and from a combined record based
on TOMS and OMI satellite datasets with gaps filled by MSR-2 (1993–1995)
are considered in the study. Ozone trends are computed by a piece-wise
trend (PWT) proxy  that includes two linear functions before and after the
turnaround year in 2001 and a parabolic function to account for the
saturation of the polar ozone destruction. In order to evaluate average total
ozone within the vortex, two classification methods are used, based on the
potential vorticity gradient as a function of equivalent latitude. The first
standard one considers this gradient at a single isentropic level (475  or
550 K), while the second one uses a range of isentropic levels between 400
and 600 K. The regression model includes a new proxy (GRAD) linked to the
gradient of potential vorticity as a function of equivalent latitude and
representing the stability of the vortex during the studied month. The
determination coefficient (<inline-formula><mml:math id="M1" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>) between observations and modelled values
increases by <inline-formula><mml:math id="M2" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 0.05 when this proxy is included in the MLR
model. Highest <inline-formula><mml:math id="M3" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> (0.92–0.95) and minimum residuals are obtained for the
second classification method for both datasets and months.</p>
    <p id="d1e213">Trends in September over the 2001–2017 period are statistically
significant at 2<inline-formula><mml:math id="M4" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> level with values ranging between 1.84 <inline-formula><mml:math id="M5" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.03
and 2.83 <inline-formula><mml:math id="M6" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.48 DU yr<inline-formula><mml:math id="M7" 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> depending on the methods and considered
proxies. This result confirms the recent studies of Antarctic ozone healing
during that month. Trends from 2001 are 2 to 3 times smaller than before the
turnaround year, as expected from the response to the slowly ozone-depleting
substances decrease in polar regions.</p>
    <p id="d1e249">For the first time, significant trends are found for the period of maximum
ozone depletion. Estimated trends from 2001 for the 15 September–15 October period over
2001–2017 vary from 1.21 <inline-formula><mml:math id="M8" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.83 to 1.96 DU <inline-formula><mml:math id="M9" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.99 yr<inline-formula><mml:math id="M10" 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> and
are significant at 2<inline-formula><mml:math id="M11" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> level.</p>
    <p id="d1e285">MLR analysis is also applied to the ozone mass deficit (OMD) metric for both
periods, considering a threshold at 220 DU and total ozone columns south of
60<inline-formula><mml:math id="M12" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S. Significant trend values are observed for all cases and
periods. A decrease of OMD of 0.86 <inline-formula><mml:math id="M13" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.36  and 0.65 <inline-formula><mml:math id="M14" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.33 Mt yr<inline-formula><mml:math id="M15" 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>
since 2001 is observed in September and 15 September–15 October,
respectively.</p>
    <p id="d1e323">Ozone recovery is also confirmed by a steady decrease of the relative area
of total ozone values lower than 175 DU within the vortex in the
15 September–15 October period<?pagebreak page7558?> since 2010 and a delay in the occurrence of ozone levels
below 125 DU since 2005.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p id="d1e333">The evolution of total ozone content (TOC) in Antarctica during austral
spring is strongly linked to the important stratospheric ozone decline that
was highlighted for the first time by Chubachi et al. (1985)
and Farman et al. (1985). Nowadays the photochemical and microphysical
processes leading to the massive and seasonal destruction of ozone in polar
regions are well understood. The latest Ozone Assessment Reports (WMO, 2007,
2011, 2014) have confirmed the stabilization of ozone loss in Antarctica
since 2000. The challenge now is to assess the impact of the observed
reduction in the concentration of ozone-depleting substances (ODSs)
(evaluated in the polar regions to <inline-formula><mml:math id="M16" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 10 % in 2013 from the peak
values in 2000; WMO, 2014) on the amplitude of the ozone destruction every
year. During the last decade, several studies have been carried out to
quantify a possible increase in total ozone column in the Antarctic polar
vortex in spring directly linked to this decrease in the polar stratosphere.
Most analyses use multilinear regression (MLR) models with different proxies
to represent the interannual variability of ozone as a function of the
11-year solar cycle, the quasi-biennial oscillation (QBO), volcanic aerosols
(Aer) or eddy heat flux (HF) (Salby et al., 2012; Kuttippurath et al., 2013;
de Laat et al., 2015). These studies generally show a significant increase of
TOC since 2000 for the September–November averaged period but they differ on
the proxies used for the quantification of ozone interannual variability.
De Laat et al. (2015) used a “big data” ensemble approach to calculate
trends. Several scenarios were considered for the period over which the ozone
record is calculated and for the different proxy records. They found that the
significance of trends could vary from negligible to 100 % significant at
2<inline-formula><mml:math id="M17" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> levels depending on the scenario considered. They have also
determined the optimal proxy records and ozone record scenarios to obtain the
best regression. The limitation of MLR analysis is that only formal
statistical error of trend is estimated and structural uncertainties linked
to the single and arbitrary combination of proxies is not taken into account.
De Laat et al. (2017) inferred trend values from daily ozone mass deficit
(OMD) computed from a multi-sensor reanalysis (MSR) dataset without using any
model but filtering the anomalous years with low polar stratospheric cloud
(PSC) volume. The authors found positive and highly significant trend of OMD
since 2000.</p>
      <p id="d1e350">Solomon et al. (2016) evaluated trends in total ozone and ozone profiles
records as well as healing characteristics by combining measurements
(satellites and ozonesondes) and the Specified Dynamics version of the Whole
Atmosphere Community Climate Model (SD-WACCM). They found a significant
healing in September but not in October, during which ozone depletion is largest
in the first 2 weeks. They also explain the difficulty of estimating
the trend in October because the large variability of ozone linked to temperature
variations and transport. The baroclinicity of the polar vortex in October
and its displacement from the geographic pole can also contribute to the
variability of the total ozone series averaged during the month of October.</p>
      <p id="d1e353">The direct link observed between positive trends of total ozone within the
polar vortex and the reduction of ODSs remains
open to debate, given the natural variability of the Antarctic vortex and
the possible contribution of greenhouse gases  to the trends
(Chipperfield et al., 2017).</p>
      <p id="d1e356">The purpose of this paper is to provide an update of the ozone
evolution inside the Antarctic vortex during the last decades, taking into
account the vortex baroclinicity. The main aim is to determine the different
contributions to ozone interannual variability and to estimate the post-2001 total ozone trend and related significance for different periods:
September, which corresponds to the period of fastest development of
catalytic photochemical ozone destruction, and mid-September to mid-October
when the maximum ozone loss is reached.</p>
      <p id="d1e360">This paper is organized as follows. Ozone datasets from satellites and
MSR are presented in Sect. 2 and the description of the
method used for total ozone column classification inside the vortex in Sect. 3.
The influence of vortex baroclinicity on total ozone column inside the
vortex is assessed in Sect. 4 by using a new classification method compared
to standard ones based on a single isentropic level. Ozone trends before and
after  the turnaround year calculated using a multi-regression model
for September and mid-September to mid-October are presented and discussed
in Sect. 5. Results of trends using OMD records as a metric are also
presented. The temporal evolution of the amount of very low total ozone
values inside the vortex is evaluated in Sect. 6. Conclusions are finally
presented in Sect. 7.</p>
</sec>
<sec id="Ch1.S2">
  <title>Total ozone column data series</title>
      <p id="d1e369">Total ozone global fields from satellite observations – Total Ozone Mapping Spectrometer
(TOMS) and Ozone Monitoring Instrument (OMI) –
and MSR are used in this study to cross-check
trend estimation before and after a turnaround year over the 1980–2017
period.</p>
<sec id="Ch1.S2.SS1">
  <title>Space-borne observations</title>
      <p id="d1e377">Total ozone column data series of NASA's TOMS instrument on board Nimbus-7 (N7) and Earth Probe (EP) between 1980 and
2004 are used. The instrument is a single monochromator that was designed for
near-nadir measurements of the total ozone column (e.g. McPeters et al.,
1998). TOMS measures the backscattering of solar radiation by the<?pagebreak page7559?> Earth's
atmosphere in six 1 nm bands of ultraviolet wavelength between 306  to 380 nm,
more or less absorbed by ozone. Total ozone column is inferred from the
ratio of two wavelengths, 317.5 nm strongly absorbed by ozone and 331.2 nm
weakly absorbed (Bhartia and Wellemeyer, 2002). Level 3 gridded TV8 data of
1.0<inline-formula><mml:math id="M18" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> (lat) <inline-formula><mml:math id="M19" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1.25<inline-formula><mml:math id="M20" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> (long) of total ozone columns of
TOMS were used in this work and are available from the Goddard Earth Sciences
Distributed Information and Services Center (GES DISC) in simple ASCII format
in the NASA anonymous ftp site
(<uri>ftp://toms.gsfc.nasa.gov/</uri>, last access:   27 May 2018)</p>
      <p id="d1e408">Ozone total column observations of OMI on board
Aura satellite are also used to continue TOMS measurements from 2005 to 2017.
The OMI instrument is a nadir-viewing hyperspectral imaging in a push-broom
mode. OMI measures the solar backscatter radiation in the complete spectrum
of the ultraviolet–visible wavelength range (270–500 nm) with 0.5 nm
spectral resolution (Levelt et al., 2006). Total ozone column used in this
work was retrieved using TV8 algorithm, hereafter referred to as OMIT in
order to maintain continuity with TOMS data record (McPeters et al., 2008).
Level 3 daily gridded data of OMI with better spatial resolution
(1.0<inline-formula><mml:math id="M21" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M22" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1.0<inline-formula><mml:math id="M23" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>) than TOMS are used. Data are also available on
NASA's anonymous ftp site.</p>
      <p id="d1e436">The total ozone column data series was combined by using specific satellite
data over the following periods: TOMS-N7 (1980–1992), TOMS-EP (1996–2004) and
OMI (2005–2017). Note that data of 1993–1995 are sparse or missing for the
September–October period. In order to complete the data series, total ozone
columns of Multi-Sensor Reanalysis version 2 (MSR-2) were used (see Sect. 2.2). Since TOMS and OMI UV
sensors do not receive enough UV light in early September, originating from
regions not illuminated by the Sun (from 77  to 82.5<inline-formula><mml:math id="M24" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S up
to mid-September), these regions were not considered to compute the total
ozone mean value in MSR-2 data.</p>
      <p id="d1e448">TOMS, OMI and MSR-2 data series have previously been used in different
scientific studies of ozone recovery in the southern polar region (Salby et
al., 2012; Kuttippurath et al., 2013; Solomon et al., 2016). Hereafter the
1980–2017 composite satellite total ozone series will be called SAT.</p>
</sec>
<sec id="Ch1.S2.SS2">
  <title>Multi-sensor reanalysis</title>
      <p id="d1e457">Ozone MSR-2 provides global assimilated ozone fields for the period
1980–2017 based on 14 satellite datasets (van der A et al., 2015). The 14
polar-orbiting satellites measuring in the near-ultraviolet Huggins band were
corrected to construct a merged satellite data series that are assimilated
within the chemistry–transport assimilation model TM3-DAM to obtain MSR-2
data (see van der A et al., 2010, for a detailed description and van der A et
al., 2015, for last improvements of the assimilation model). Corrections of
offset, trends and variations of solar zenith angle and temperature in the
stratosphere were computed in satellite datasets by comparisons with
individual ground-based Dobson and Brewer measurements from World Ozone and
Ultraviolet Data Center (WOUDC). Those corrections are specified in van der A
et al. (2015), Table 2.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><caption><p id="d1e463">Information of proxies (source, characteristics and time window for
the mean yearly value).</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="justify" colwidth="199.169291pt"/>
     <oasis:colspec colnum="3" colname="col3" align="justify" colwidth="170.716535pt"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Proxy</oasis:entry>
         <oasis:entry colname="col2">Source</oasis:entry>
         <oasis:entry colname="col3">Characteristics</oasis:entry>
         <oasis:entry colname="col4">Time window</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">HF</oasis:entry>
         <oasis:entry colname="col2">NASA's Goddard Space Flight Center <?xmltex \hack{\hfill\break}?> <uri>https://acd-ext.gsfc.nasa.gov/Data_services/met/ann_data.html</uri> (last access: 27 May 2018)</oasis:entry>
         <oasis:entry colname="col3">45-day mean heat flux between 45 and 75<inline-formula><mml:math id="M25" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S at 70 hPa from MERRA 2</oasis:entry>
         <oasis:entry colname="col4">Aug–Sept</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">SF</oasis:entry>
         <oasis:entry colname="col2">Dominion Radio Astrophysical Observatory (National Research Council Canada) <?xmltex \hack{\hfill\break}?> <uri>ftp://ftp.geolab.nrcan.gc.ca/data/solar_flux/monthly_averages/solflux_monthly_average.txt</uri> (last access: 27 May 2018)</oasis:entry>
         <oasis:entry colname="col3">Monthly averages of solar flux at 10.7 cm <?xmltex \hack{\hfill\break}?>wavelength</oasis:entry>
         <oasis:entry colname="col4">Sep</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">QBO</oasis:entry>
         <oasis:entry colname="col2">Institute of Meteorology (Freie Universität Berlin) <?xmltex \hack{\hfill\break}?> <uri>http://www.geo.fu-berlin.de/en/met/ag/strat/produkte/qbo</uri> (last access: 27 May 2018)</oasis:entry>
         <oasis:entry colname="col3">Monthly mean quasi-biennial oscillation at <?xmltex \hack{\hfill\break}?>30 and 10 hPa</oasis:entry>
         <oasis:entry colname="col4">Sep</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Aer</oasis:entry>
         <oasis:entry colname="col2">1980–1990: NASA's Goddard Space Flight Center <?xmltex \hack{\hfill\break}?> <uri>https://data.giss.nasa.gov/modelforce/strataer/</uri> (last access: 27 May 2018) <?xmltex \hack{\hfill\break}?>Jan 1991–Apr 2017 composite data series <?xmltex \hack{\hfill\break}?></oasis:entry>
         <oasis:entry colname="col3">AOD at 550nm; 15–30 km; 40–65<inline-formula><mml:math id="M26" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S zonal<?xmltex \hack{\hfill\break}?>mean <?xmltex \hack{\hfill\break}?>AOD at 532nm merged satellite time series of SAGE II, OSIRIS, CALIOP and OMPS following method described in Khaykin et al. (2017) <?xmltex \hack{\hfill\break}?>15–30 km; 40–65<inline-formula><mml:math id="M27" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S zonal mean</oasis:entry>
         <oasis:entry colname="col4">Apr</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">AAO</oasis:entry>
         <oasis:entry colname="col2">NOAA's National Weather Service <?xmltex \hack{\hfill\break}?> <uri>ftp://ftp.cpc.ncep.noaa.gov/cwlinks/</uri> (last access: 27 May 2018)</oasis:entry>
         <oasis:entry colname="col3">Daily AAO index</oasis:entry>
         <oasis:entry colname="col4">Same as <inline-formula><mml:math id="M28" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">GRAD</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">Daily maximum of PV slope at 550 K computed from ERA-Interim data</oasis:entry>
         <oasis:entry colname="col4">Same as <inline-formula><mml:math id="M29" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T2"><caption><p id="d1e679">Coefficient of determination <inline-formula><mml:math id="M30" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> and trends <inline-formula><mml:math id="M31" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>2<inline-formula><mml:math id="M32" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> in
DU yr<inline-formula><mml:math id="M33" 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> before and after the turnaround year 2001 derived from
multi-regression model using as input MSR-2 (1980–2017) total ozone
anomalies inside the vortex for September using three classification methods
described in Sect. 3.2. The residual is represented in  DU by <inline-formula><mml:math id="M34" display="inline"><mml:mrow><mml:mi mathvariant="italic">χ</mml:mi><mml:mo>=</mml:mo><mml:msqrt><mml:mrow><mml:msub><mml:mo>∑</mml:mo><mml:mi>i</mml:mi></mml:msub><mml:msup><mml:mfenced close=")" open="("><mml:mrow><mml:msub><mml:mi mathvariant="normal">obs</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="normal">mod</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:mfenced><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>/</mml:mo><mml:mo>(</mml:mo><mml:mi>n</mml:mi><mml:mo>-</mml:mo><mml:mi>m</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:msqrt></mml:mrow></mml:math></inline-formula>, where obs<inline-formula><mml:math id="M35" display="inline"><mml:msub><mml:mi/><mml:mi>i</mml:mi></mml:msub></mml:math></inline-formula>
and mod<inline-formula><mml:math id="M36" display="inline"><mml:msub><mml:mi/><mml:mi>i</mml:mi></mml:msub></mml:math></inline-formula> correspond to observations and model
monthly mean, <inline-formula><mml:math id="M37" display="inline"><mml:mi>n</mml:mi></mml:math></inline-formula> the number of years and <inline-formula><mml:math id="M38" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula> the number of parameters fitted as
in Weber et al. (2018).</p></caption><oasis:table frame="topbot"><?xmltex \begin{scaleboxenv}{.92}[.92]?><oasis:tgroup cols="4">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry namest="col2" nameend="col4" align="center">Multi-sensor reanalysis (MSR-2) </oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">400–600 K</oasis:entry>
         <oasis:entry colname="col3">475 K</oasis:entry>
         <oasis:entry colname="col4">550 K</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M39" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.92</oasis:entry>
         <oasis:entry colname="col3">0.90</oasis:entry>
         <oasis:entry colname="col4">0.92</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend before 2001</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M40" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.31 <inline-formula><mml:math id="M41" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.67</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M42" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>4.90 <inline-formula><mml:math id="M43" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.74</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M44" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.23 <inline-formula><mml:math id="M45" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.68</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend after 2001</oasis:entry>
         <oasis:entry colname="col2">1.84 <inline-formula><mml:math id="M46" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.03</oasis:entry>
         <oasis:entry colname="col3">2.36 <inline-formula><mml:math id="M47" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.16</oasis:entry>
         <oasis:entry colname="col4">1.92 <inline-formula><mml:math id="M48" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.07</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"><inline-formula><mml:math id="M49" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">10.74</oasis:entry>
         <oasis:entry colname="col3">12.02</oasis:entry>
         <oasis:entry colname="col4">11.12</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry namest="col2" nameend="col4" align="center">Only with GRAD, HF and PWT </oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M50" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.91</oasis:entry>
         <oasis:entry colname="col3">0.89</oasis:entry>
         <oasis:entry colname="col4">0.89</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend before 2001</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M51" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.32 <inline-formula><mml:math id="M52" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.64</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M53" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.00 <inline-formula><mml:math id="M54" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.71</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M55" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.21 <inline-formula><mml:math id="M56" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.70</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend after 2001</oasis:entry>
         <oasis:entry colname="col2">1.91 <inline-formula><mml:math id="M57" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.94</oasis:entry>
         <oasis:entry colname="col3">2.26 <inline-formula><mml:math id="M58" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.04</oasis:entry>
         <oasis:entry colname="col4">2.00 <inline-formula><mml:math id="M59" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.04</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"><inline-formula><mml:math id="M60" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">10.61</oasis:entry>
         <oasis:entry colname="col3">11.82</oasis:entry>
         <oasis:entry colname="col4">11.71</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry namest="col2" nameend="col4" align="center">Only with HF and PWT </oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M61" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.84</oasis:entry>
         <oasis:entry colname="col3">0.77</oasis:entry>
         <oasis:entry colname="col4">0.82</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend before 2001</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M62" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.34 <inline-formula><mml:math id="M63" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.84</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M64" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>4.79 <inline-formula><mml:math id="M65" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.97</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M66" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.23 <inline-formula><mml:math id="M67" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.89</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend after 2001</oasis:entry>
         <oasis:entry colname="col2">2.04 <inline-formula><mml:math id="M68" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.24</oasis:entry>
         <oasis:entry colname="col3">2.83 <inline-formula><mml:math id="M69" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.48</oasis:entry>
         <oasis:entry colname="col4">2.13 <inline-formula><mml:math id="M70" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.31</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M71" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">14.04</oasis:entry>
         <oasis:entry colname="col3">16.03</oasis:entry>
         <oasis:entry colname="col4">14.81</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup><?xmltex \end{scaleboxenv}?></oasis:table></table-wrap>

      <p id="d1e1261">Daily gridded forecast ozone data of MSR-2 at 12:00 UTC and spatial resolution
of 0.5<inline-formula><mml:math id="M72" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M73" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.5<inline-formula><mml:math id="M74" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> were used in this work and they are
available from the Tropospheric Emission Monitoring Internet Service (TEMIS)
of KNMI/ESA (<uri>http://www.temis.nl/protocols/o3field/data/msr2/</uri>, last access: 27 May 2018).</p>
      <p id="d1e1292">Different studies on trends in the Southern Hemisphere have used MSR-2 data
(Kuttippurath et al., 2013; de Laat et al., 2015,  2017). Hereafter the
1980–2017 ozone series will be called MSR-2.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <title>Data classification within the vortex</title>
      <p id="d1e1302">In order to consider total ozone columns only within the polar vortex, the
data classification is performed by evaluating the vortex's position at
different isentropic levels from 1 May  to 31 December, each year. Two
classification methods are then applied in order to evaluate the impact of
baroclinicity of the vortex on the averaged total ozone columns in both
studied depletion periods. The first one is based on a single isentropic
level, while the second one considers a range of isentropic levels.</p>
<sec id="Ch1.S3.SS1">
  <title>Vortex position</title>
      <p id="d1e1310">For each day of the studied periods, the vortex position is determined by
using a 2-D quasi-conservative coordinate system (equivalent
latitude–potential temperature) described by McIntyre and Palmer (1984), where
the pole in equivalent latitude (EL) corresponds to the position of maximum
potential vorticity (PV). This conservative system is computed from PV field
simulated by the Modélisation Isentrope du transport Mésoéchelle
de l'Ozone Stratosphérique par Advection (MIMOSA) PV advection model
(Hauchecorne et al., 2002). The model was forced by ERA-Interim (Dee et al.,
2011) meteorological data (2.5<inline-formula><mml:math id="M75" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M76" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 2.5<inline-formula><mml:math id="M77" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>) of European
Centre for Medium-Range Weather Forecasts (ECMWF). Daily advected PV fields
(1<inline-formula><mml:math id="M78" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M79" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1<inline-formula><mml:math id="M80" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>) on the 30–90<inline-formula><mml:math id="M81" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S
latitude band at 12:00 UTC are used to calculate EL on the isentropic level
range between 400 and 600 K with a step of 25 K.</p>
      <p id="d1e1373">Following Nash et al. (1996), PV is evaluated as a function of EL and three
particular regions are identified: inside the vortex, characterized by high
PV values, at the vortex edge, corresponding to high PV gradients and
outside the vortex (or surf zone) with small PV values. The limit of the
vortex corresponds to the EL of maximum PV gradient, weighted by the wind
module. This limit is subsequently smoothed temporally with a moving average
of 5 days to reduce the noise in the vortex edge data series.</p><?xmltex \hack{\newpage}?>
</sec>
<?pagebreak page7560?><sec id="Ch1.S3.SS2">
  <title>Methodology for classification</title>
      <p id="d1e1383">The Nash criterion was already used in several studies to distinguish
measurements (ozone profiles and total columns) inside and outside the
vortex in the Southern Hemisphere (Godin et al., 2001; Bodeker et al., 2002;
Pazmiño et al., 2005, 2008; Kuttippurath et al., 2013, 2015). In the case of
total columns, measurements were considered inside the vortex when their
corresponding EL was larger than the EL of the vortex limit at a specific
isentropic level (e.g. 550 K, Bodeker et al., 2002; Pazmiño et al., 2005).
However, this “standard” method does not take into account the
baroclinicity of the vortex. It can result in the classification of total
ozone columns inside the vortex while partial columns below or above the
selected isentropic level are outside the vortex. The total ozone column may
thus not represent the ozone behaviour inside the vortex. In order to
consider possible vortex baroclinicity, another approach is used, where
vortex classification at different isentropic levels is considered at the
same time. For this second approach, the range of selected isentropic levels
is chosen in the altitude region of maximum ozone depletion: from 400  to
600 K with a step of 25 K. The same nine isentropic levels considered for
400–600 K range classification are applied each year.</p>
      <p id="d1e1386">In order to illustrate the impact of vortex baroclinicity on the
classification of total ozone column inside the vortex, Fig. 1 shows MSR-2
total ozone fields on 7 October   2012, with the vortex position computed at
different isentropic levels superimposed. The vortex position curves are
represented by black to light grey colours. On this particular day, the
region classified inside the vortex in the 400–600 K range is limited by
the vortex position at 400 K (black line) towards west Antarctic coast and
Palmer Peninsula and at 600 K (light grey line) towards the east Antarctic
coast. The white dot marks in Fig. 1 show the limit of the region considered
in this new classification. In the case of standard classification using a
single level at 475  or 550 K, the region estimated as inside the vortex
consists of an area with total ozone columns larger than 400 DU. These areas
are not considered in the classification using several isentropic levels
between 400  and 600 K. Regions where total ozone columns are lower than
220 DU are taken into account by the classification at all the isentropic
levels. A daily mean total ozone column of 213.4 DU was computed inside the
vortex using this new classification method. The standard classification
estimates a 40  and 20 DU larger ozone average values at 475 and 550 K,
respectively, on that day.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><caption><p id="d1e1391">Total
ozone (DU) from MSR-2 on 7 October   2012 at 12:00 UTC. Vortex
edge position at different isentropic levels are added to the map and
represented by black to light grey lines. White dot marks identify the
region considered inside the vortex using the 400–600 K range
classification.</p></caption>
          <?xmltex \igopts{width=199.169291pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f01.png"/>

        </fig>

</sec>
</sec>
<sec id="Ch1.S4">
  <title>Vortex baroclinicity</title>
      <p id="d1e1407">Both methods of classification described in the previous section were
applied to satellite composite total ozone data<?pagebreak page7561?> series SAT and MSR-2
reanalysis at each grid point. For each year, daily mean total ozone amount
inside the vortex was averaged over two periods: the whole month of
September and the period of maximum ozone depletion between
15 September and 15 October. Figure 2 shows the evolution
of total ozone average inside the vortex for the 15 September–15 October period between
1980 and 2017 for the MSR-2 data series computed with the standard
classification method based on the single isentropic level (475  and 550 K)
and with the second method using the 400–600 K range of isentropic
levels. Error bars represent the 2<inline-formula><mml:math id="M82" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> standard error.
Similar interannual total ozone variability is observed for the time series
obtained by the different methods. The correlation coefficients between the
range method and the standard one at 475  and 550 K are 0.98 and 0.99,
respectively. Despite these good correlations, the data series are
significantly different at the 2<inline-formula><mml:math id="M83" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> level. Larger ozone values are
found with the standard method, especially for the 475 K level, which shows
a mean difference with the TOC time series based on the range method
of <inline-formula><mml:math id="M84" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 15 % over the whole analysis period. Three years stand
out in the comparison – 1995, 1999 and 2011 – during which the inside vortex
region was systematically larger at 475 K compared to higher isentropic
levels during the period. Similar results are observed for September (not
shown). In this work, the second method is preferred since it takes into
account the ozone loss at different isentropic levels, which strongly
impacts the total column.</p>
      <p id="d1e1431">MSR-2 total ozone time series obtained in September and 15 September–15 October with the
range classification method are displayed in Fig. 3. September presents
<inline-formula><mml:math id="M85" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 8 % larger ozone mean values than the 15 September–15 October period.
Similar interannual variability is observed between the two periods as shown
by the correlation coefficient of 0.98. The last 4 years present very
similar ozone values of around 205 DU in September, while during the 15 September–15 October period
they show larger variability.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><caption><p id="d1e1443">Evolution of total ozone of MSR-2 dataset inside the vortex
averaged each year on 15 September–15 October period for different classifications:
standard method at 475 and 550 K represented by black and blue lines,
respectively, and method considering the 400–600 K altitude range by the red
line. Error bars represent twice the standard error.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f02.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><caption><p id="d1e1455">As in Fig. 2 but only for 400–600 K classification on different
periods: September and mid-September to mid-October. Error bars represent
2<inline-formula><mml:math id="M86" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f03.png"/>

      </fig>

      <p id="d1e1471">MSR-2 total ozone data series inside the vortex are compared to SAT series
as shown in Fig. 4, which displays the relative difference between MSR-2 and
SAT for the 400–600 K range classification. Differences of about <inline-formula><mml:math id="M87" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.5 %
are observed in the 1980s. Small differences are expected during
this period since only TOMS data are used in both datasets until 1993. In
the 1993–1995 period discrepancies between both curves are only due to the
differences in the selection of MSR-2 data for the SAT record in order to
have similar spatial coverage as the data from the other instruments
incorporated in the SAT time series. These differences varying between <inline-formula><mml:math id="M88" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1
and 0.5 % represent an estimation of the impact of reduced spatial
coverage in SAT dataset on the averaged total ozone level in September. The
15 September–15 October period presents negligible differences. The addition of GOME
(1996–2005) in MSR-2 assimilation could explain the discrepancies with the
SAT dataset that considers only TOMS-EP. From 2001, differences are larger
and generally positive, reaching <inline-formula><mml:math id="M89" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 5 % in September and
<inline-formula><mml:math id="M90" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 3 % in the 15 September–15 October period. These increased differences
are especially visible during the period where data from instruments on
board the ENVISAT platform (e.g.<?pagebreak page7562?> SCIAMACHY) are assimilated in the MSR-2
record. Overall, values in September present a mean bias of 1.3 % (dash
blue line in Fig. 4) and during 15 September–15 October a smaller bias value of 0.5 %
(dash red line in Fig. 4). Temporal evolution of the differences, e.g.
negative trend in the 1980s and positive trend in the 2000s, can have an
impact on the long-term ozone trends retrieved from both records. In
general, differences between SAT and MSR-2 records are caused by MSR-2
starting to use multiple satellite total ozone columns records after 1996,
procedures in MSR-2 to account for inter-instrument differences and
data assimilation methodology that allows for filling gaps (van der A et
al., 2015).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><caption><p id="d1e1504">Relative difference between MSR-2 and SAT mean total ozone inside
the vortex for September (blue curve) and 15 September–15 October (red curve) periods.
Horizontal dash lines correspond to the mean bias between data series.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f04.png"/>

      </fig>

      <p id="d1e1513">Despite the differences between those datasets, one purpose of this work was
to analyse, in the same way, satellite data such as those included in the SAT
record without any correction or adjustment and the MSR-2 record, which
accounts for inter-instrument differences using ground-based total column
data. Due to the larger differences observed between both datasets in
September, especially in the 1995–2010 period, which may have an impact on
trend analysis, it was decided to retrieve trends from the SAT dataset in
the 15 September–15 October only.</p>
      <p id="d1e1516">In the next section, ozone data series based on the different classification
methods are used to evaluate the impact of vortex baroclinicity on ozone
trends inside the vortex for both studied periods.</p>
</sec>
<sec id="Ch1.S5">
  <title>Trend analysis</title>
<sec id="Ch1.S5.SS1">
  <title>Method</title>
      <p id="d1e1531">In order to evaluate ozone recovery in Antarctica, estimation of trends
before and after 2001 were calculated using a multi-regression model (Nair
et al., 2013) updated from the AMOUNTS (Adaptative Model for Unambiguous
Trend Survey) model (Hauchecorne et al., 1991; Kerzenmacher et al., 2006).
Different common explanatory variables such as eddy HF, solar
flux (SF), QBO, Aer and Antarctic
oscillation (AAO) are used to explain total ozone variability over the
1980–2017 period. These proxies were widely applied in different trend
studies (e.g. de Laat et al., 2015, and references herein). The ODS
contribution to long-term trend in ozone is represented by piece-wise trend (PWT)
functions. The total ozone variability (<inline-formula><mml:math id="M91" display="inline"><mml:mi>Y</mml:mi></mml:math></inline-formula>) can be expressed
following Eq. (1):

                <disp-formula specific-use="align" content-type="numbered"><mml:math id="M92" display="block"><mml:mtable displaystyle="true"><mml:mtr><mml:mtd><mml:mstyle class="stylechange" displaystyle="true"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mi>Y</mml:mi><mml:mfenced open="(" close=")"><mml:mi>t</mml:mi></mml:mfenced><mml:mo>=</mml:mo><mml:mi>K</mml:mi><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">HF</mml:mi></mml:msub><mml:mi mathvariant="normal">HF</mml:mi><mml:mfenced open="(" close=")"><mml:mi>t</mml:mi></mml:mfenced><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">SF</mml:mi></mml:msub><mml:mi mathvariant="normal">SF</mml:mi><mml:mfenced open="(" close=")"><mml:mi>t</mml:mi></mml:mfenced><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi mathvariant="normal">QBO</mml:mi><mml:mn mathvariant="normal">30</mml:mn></mml:mrow></mml:msub><mml:mi mathvariant="normal">QBO</mml:mi><mml:mn mathvariant="normal">30</mml:mn><mml:mfenced open="(" close=")"><mml:mi>t</mml:mi></mml:mfenced></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi mathvariant="normal">QBO</mml:mi><mml:mn mathvariant="normal">10</mml:mn></mml:mrow></mml:msub><mml:mi mathvariant="normal">QBO</mml:mi><mml:mn mathvariant="normal">10</mml:mn><mml:mfenced open="(" close=")"><mml:mi>t</mml:mi></mml:mfenced><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">Aer</mml:mi></mml:msub><mml:mi mathvariant="normal">Aer</mml:mi><mml:mfenced open="(" close=")"><mml:mi>t</mml:mi></mml:mfenced><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">AAO</mml:mi></mml:msub><mml:mi mathvariant="normal">AAO</mml:mi><mml:mfenced open="(" close=")"><mml:mi>t</mml:mi></mml:mfenced></mml:mrow></mml:mtd></mml:mtr><mml:mlabeledtr id="Ch1.E1"><mml:mtd/><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">GRAD</mml:mi></mml:msub><mml:mi mathvariant="normal">GRAD</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mi mathvariant="normal">PWT</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mo>∈</mml:mo><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

            where <inline-formula><mml:math id="M93" display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula> is year from 1980 to 2017, <inline-formula><mml:math id="M94" display="inline"><mml:mi>K</mml:mi></mml:math></inline-formula> is a
constant, <inline-formula><mml:math id="M95" display="inline"><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mi mathvariant="normal">proxy<?pagebreak page7563?></mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> are the regression coefficients of the
respective proxies mentioned above and <inline-formula><mml:math id="M96" display="inline"><mml:mrow><mml:mo>∈</mml:mo><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> is the total ozone
residuals. Table 1 shows the respective information for each proxy: source,
specific characteristics and time window where proxy values are averaged to
represent the respective year value. QBO effect on ozone variability is
estimated using two proxies at 30 hPa (QBO30) and 10 hPa (QBO10), which are
out of phase by <inline-formula><mml:math id="M97" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mi mathvariant="italic">π</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mfrac></mml:mstyle></mml:mrow></mml:math></inline-formula> (Steinbrecht et al., 2003). The HF
proxy corresponds to the average over the August–September period of the
45-day mean heat flux in the 45–75<inline-formula><mml:math id="M98" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S latitude range at 70 hPa
from MERRA-2 analyses. The time window of August–September is selected for
computing the mean HF, following de Laat et al. (2015) recommendation to
obtain the best regression results. For the Aer term, a merged proxy of
monthly aerosol optical depth (AOD) is computed from updated Sato et
al. (1993) dataset for the 1980–1990 period and from four satellite data
series (SAGE II, OSIRIS, CALIOP and OMPS) for the 1991–2017 period. AOD
datasets are averaged over the 40–65<inline-formula><mml:math id="M99" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S zonal region in the
15–30 km altitude range. Updated Sato et al. data are obtained from NASA
monthly AOD at 550 nm. The satellite AOD data over 1991–2017 period were
computed at 532 nm. The Sato et al. dataset was converted to 532 nm
according to Khaykin et al. (2017). The merged AOD proxy was obtained by
normalizing the Sato et al. time series to the SAGE II data in December 1991.
The regression code uses the AOD values in April before the complete
formation of the vortex in order to avoid possible contamination of aerosols
satellite data by PSCs. The April AOD proxy is represented by a bold black
line in Fig. 5 together with Sato et al. (1993) and satellites datasets for
the 1991–2017 period.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><caption><p id="d1e1771">Time series of April monthly mean AOD at 532 nm within 40–65<inline-formula><mml:math id="M100" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S
and 15–30 km of normalized Sato et al. (1993) dataset (see
main text) and from satellites (SAGE II, OSIRIS, CALIOP, OMPS). The
corresponding merged data are represented by the bold line.</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f05.png"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6"><caption><p id="d1e1791">Heat flux <bold>(a)</bold> and gradient (GRAD) <bold>(b)</bold> anomalies
for the 15 September–15 October period: before removing a polynomial fit of
third
order (black line), the fit (grey line) and after removing the fit (blue/red
line).</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f06.png"/>

        </fig>

      <p id="d1e1807">A new GRAD(<inline-formula><mml:math id="M101" display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula>) proxy was developed in order to take into account the
stability of the vortex during the studied period. This proxy corresponds to
the maximum gradient of PV as a function of EL at 550 K during both studied
periods (e.g. September and 15 September–15 October). It is calculated from ERA-Interim
data. GRAD and HF proxies are detrended by removing a third-order
polynomial fit to minimize correlation with PWT proxies. Figure 6 displays
GRAD and HF proxies before and after removing trends. An anticorrelation of
<inline-formula><mml:math id="M102" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 0.55 between these two proxies is observed with a <inline-formula><mml:math id="M103" display="inline"><mml:mi>p</mml:mi></mml:math></inline-formula> value &lt; 0.01,
but the addition of GRAD proxy provides a much better
agreement between measurements and model, especially during the last decade.
The contribution of the GRAD(<inline-formula><mml:math id="M104" display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula>) proxy to the improvement of the MLR results
is discussed in Sect. 5.2.3.</p>
      <p id="d1e1838">For the long-term trends, two piece-wise linear trend <inline-formula><mml:math id="M105" display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mi mathvariant="normal">PWLT</mml:mi><mml:mfenced close=")" open="("><mml:mi>t</mml:mi></mml:mfenced><mml:mo>=</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msub><mml:mi>t</mml:mi><mml:mn mathvariant="normal">1</mml:mn><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub><mml:mi>t</mml:mi><mml:mn mathvariant="normal">2</mml:mn><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> functions
calculated before and after the turnaround year are usually used to estimate
the change of slope in the long-term evolution of ozone due to ODSs (e.g.
Reinsel et al., 2002; Kuttippurath et al., 2013; de Laat et al., 2015). In
this work our modified PWLT model (PWT) uses an additional function in order
to take into account the slower growth of ODSs near the turnaround year and
the ozone loss saturation effect within the Antarctic polar vortex in
October (Yang et al., 2008). The PWT model is represented by Eq. (2):
            <disp-formula id="Ch1.E2" content-type="numbered"><mml:math id="M106" display="block"><mml:mrow><mml:mi mathvariant="normal">PWT</mml:mi><mml:mfenced open="(" close=")"><mml:mi>t</mml:mi></mml:mfenced><mml:mo>=</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:msub><mml:mi>t</mml:mi><mml:mn mathvariant="normal">11</mml:mn><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:msub><mml:mi>t</mml:mi><mml:mn mathvariant="normal">12</mml:mn><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub><mml:mi>t</mml:mi><mml:mn mathvariant="normal">2</mml:mn><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
          where <inline-formula><mml:math id="M107" display="inline"><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M108" display="inline"><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> are the coefficients of the linear functions
and <inline-formula><mml:math id="M109" display="inline"><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> of the parabolic function. The first period is represented by
a linear time proxy <inline-formula><mml:math id="M110" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:math></inline-formula> and a parabolic time proxy
<inline-formula><mml:math id="M111" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:math></inline-formula>. The second period is expressed only by a linear time
proxy <inline-formula><mml:math id="M112" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>. The proxies are computed as follows:

                <disp-formula specific-use="align" content-type="numbered"><mml:math id="M113" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="Ch1.E3"><mml:mtd/><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mi>t</mml:mi><mml:mn mathvariant="normal">11</mml:mn><mml:mo>=</mml:mo><mml:mfenced close="" open="{"><mml:mtable class="array" columnalign="left left"><mml:mtr><mml:mtd><mml:mi>t</mml:mi></mml:mtd><mml:mtd><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>&lt;</mml:mo><mml:mi>t</mml:mi><mml:mo>≤</mml:mo><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>&lt;</mml:mo><mml:mi>t</mml:mi><mml:mo>≤</mml:mo><mml:msub><mml:mi>T</mml:mi><mml:mi mathvariant="normal">end</mml:mi></mml:msub></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:mfenced></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E4"><mml:mtd/><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">12</mml:mn><mml:mo>=</mml:mo><mml:mfenced close="" open="{"><mml:mtable class="array" columnalign="left left"><mml:mtr><mml:mtd><mml:mrow><mml:msup><mml:mfenced close=")" open="("><mml:mrow><mml:mi>t</mml:mi><mml:mo>-</mml:mo><mml:mfenced open="(" close=")"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:mfrac></mml:mstyle></mml:mfenced></mml:mrow></mml:mfenced><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>&lt;</mml:mo><mml:mi>t</mml:mi><mml:mo>≤</mml:mo><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mrow><mml:msup><mml:mfenced open="(" close=")"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:mfrac></mml:mstyle></mml:mfenced><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>&lt;</mml:mo><mml:mi>t</mml:mi><mml:mo>≤</mml:mo><mml:msub><mml:mi>T</mml:mi><mml:mi mathvariant="normal">end</mml:mi></mml:msub></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:mfenced></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E5"><mml:mtd/><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mi>t</mml:mi><mml:mn mathvariant="normal">2</mml:mn><mml:mo>=</mml:mo><mml:mfenced open="{" close=""><mml:mtable class="array" columnalign="left left"><mml:mtr><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>&lt;</mml:mo><mml:mi>t</mml:mi><mml:mo>≤</mml:mo><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mrow><mml:mi>t</mml:mi><mml:mo>-</mml:mo><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>&lt;</mml:mo><mml:mi>t</mml:mi><mml:mo>≤</mml:mo><mml:msub><mml:mi>T</mml:mi><mml:mi mathvariant="normal">end</mml:mi></mml:msub></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:mfenced></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

            <inline-formula><mml:math id="M114" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> corresponds to the turnaround year in the considered<?pagebreak page7564?> period. In this
work, 2001 was selected as the turnaround year when equivalent effective
stratospheric chlorine maximizes for a mean age of air of 5.5 years
(Newman et al., 2007). The corresponding value for <inline-formula><mml:math id="M115" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is 22.
<inline-formula><mml:math id="M116" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mi mathvariant="normal">end</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> corresponds to the number of years considered in the study (38 for
1980–2017). The minimum of the parabolic time proxy <inline-formula><mml:math id="M117" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:math></inline-formula> is set to
the middle of the period before the turnaround year so that the slope of the
proxy is zero on that year. In this case the coefficient of <inline-formula><mml:math id="M118" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M119" display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:msub><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>
can be considered as the linear trend before 2001. After 2001, <inline-formula><mml:math id="M120" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:math></inline-formula> and
<inline-formula><mml:math id="M121" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:math></inline-formula>
are constant and then the linear trend is given by the <inline-formula><mml:math id="M122" display="inline"><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> coefficient.
Figure 7 represents the evolution of the three piece-wise proxy anomalies
normalized by the corresponding standard deviation. The improvement using
PWT instead of PWLT is discussed in Sect. 5.2.4.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7"><caption><p id="d1e2380">Anomalies of the linear functions before and after 2001 (<inline-formula><mml:math id="M123" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:math></inline-formula> and
<inline-formula><mml:math id="M124" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>, respectively) and parabolic function (<inline-formula><mml:math id="M125" display="inline"><mml:mrow><mml:mi>t</mml:mi><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:math></inline-formula>) that correspond to the PWT
proxy (see Eqs. 2 to 5). Each proxy anomaly is normalized by the
corresponding standard deviation.</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f07.png"/>

        </fig>

</sec>
<sec id="Ch1.S5.SS2">
  <title>Trend results for the averaged total ozone column records</title>
      <p id="d1e2425">The multi-regression model described in previous section was applied to
MSR-2 total ozone anomalies time series computed as monthly total ozone–mean total ozone for the September and 15 September–15 October periods and to SAT for
the 15 September–15 October period only. Time  series of total ozone data corresponding
to the different classification methods described in Sect. 4 were also used
to evaluate the impact of vortex baroclinicity on total ozone trends.</p>
<sec id="Ch1.S5.SS2.SSS1">
  <title>September</title>
      <p id="d1e2433">A rapid decrease of ozone levels occurs within the polar vortex in Antarctica
from the last 2 weeks of August to the end of September when the necessary
sunlight to start the ozone catalytic destruction cycles is present again
above austral polar regions. Important differences in total ozone levels are
found inside the vortex between the first and second half of September, with
very low values observed mostly during the last week. Although pronounced
decrease in total ozone is observed in September, recent publications have
used ozone records obtained during this month to detect the ozone recovery
(Solomon et al., 2016; Chipperfield et al., 2017; Weber et al., 2018). Those
studies use data and/or simulations poleward of <inline-formula><mml:math id="M126" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 60<inline-formula><mml:math id="M127" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and
identify first signs of Antarctic ozone recovery for September but not yet
for October due to the larger dynamical variability during that month. In
this paper, results from our multi-regression model are evaluated and
compared to those previous publications for the September period. Figure 8
illustrates the results of the regression model described in Sect. 5.1 for
the MSR-2 total ozone data series inside the vortex using the 400–600 K
range classification. The top panel represents the deseasonalized total ozone
observations as well as the regressed ozone values. The model results
reproduce quite well the interannual variability of measurements except in
2002, when the vortex split in two parts in late September due to a major
sudden stratospheric warming (e.g. Allen et al., 2003). Likewise, the year
2000 was characterized by a large ozone hole area (OHA) in September and
yielded a relatively high value of residual of <inline-formula><mml:math id="M128" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 30 DU on that year.
Contributions of the different proxies are shown in the second to fourth
panels of Fig. 8. Fitted HF and GRAD were added (black line in second
panel of Fig. 8) due to the correlation between both proxies. The model term
linked to the HF and GRAD fitted proxy represents the second largest
contribution to total ozone interannual variability (<inline-formula><mml:math id="M129" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> 10 % of the
total variance) after the PWT proxy which contributes to about 80 % of
the total variability. Other proxies (third panel of Fig. 8) represent only
1 % of total ozone variability. Aerosol proxy contributes by
<inline-formula><mml:math id="M130" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 6 DU in 1992 and <inline-formula><mml:math id="M131" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 3 DU in 1983 due to Pinatubo and El
Chichón eruptions, respectively. Negligible impact is seen in other
years. Fitted QBO (QBO30hPa <inline-formula><mml:math id="M132" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> QBO10hPa) explains <inline-formula><mml:math id="M133" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>5 DU ozone
variability. The contributions of SF and AAO proxies are negligible.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8"><caption><p id="d1e2497">Deseasonalized total ozone inside the vortex of MSR-2 series
(meas) and regression model (model) for September using 400–600 K
classification <bold>(a)</bold>. Contributions of proxies are also shown: heat
flux (HF), gradient (GRAD) and the combination of both HF and GRAD <bold>(b)</bold>;
solar flux (SF), QBO (QBO at 30 hPa and QBO at 50 hPa), Antarctic
oscillation (AAO) and aerosol (Aer) <bold>(c)</bold>; and PWT <bold>(d)</bold>.
Ozone anomalies and contributions of proxies are given in DU.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f08.png"/>

          </fig>

      <?pagebreak page7565?><p id="d1e2518">The model explains 92 % of the ozone variability as deduced from the
determination coefficient <inline-formula><mml:math id="M134" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>. The estimated total ozone trends before
and after 2001 are <inline-formula><mml:math id="M135" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.31 <inline-formula><mml:math id="M136" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.67 DU yr<inline-formula><mml:math id="M137" 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> (<inline-formula><mml:math id="M138" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>25.2 <inline-formula><mml:math id="M139" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3.2 % decade<inline-formula><mml:math id="M140" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>
and 1.84 <inline-formula><mml:math id="M141" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.03 DU yr<inline-formula><mml:math id="M142" 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> (8.8 <inline-formula><mml:math id="M143" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4.9 % decade<inline-formula><mml:math id="M144" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, respectively. Both trends are significant (i.e.
statistically different from zero) at 2<inline-formula><mml:math id="M145" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>. The 1980–2000 period
presents larger depletion rate compared to Weber et al. (2018) (from <inline-formula><mml:math id="M146" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>12 to
<inline-formula><mml:math id="M147" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>19 % per decade depending on dataset) and comparable rate for the period
of recovery (8–10 % decade<inline-formula><mml:math id="M148" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>. Comparable values of trends are found
when the 475 K classification level is used (<inline-formula><mml:math id="M149" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>21 <inline-formula><mml:math id="M150" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3.2
and 10.1 <inline-formula><mml:math id="M151" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 5 % decade<inline-formula><mml:math id="M152" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>. The 400–600 K
classification allows us to obtain the best agreement between observations
and regressed values (larger <inline-formula><mml:math id="M153" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>) and lower <inline-formula><mml:math id="M154" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M155" display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:msqrt><mml:mrow><mml:msub><mml:mo>∑</mml:mo><mml:mi>i</mml:mi></mml:msub><mml:msup><mml:mfenced open="(" close=")"><mml:mrow><mml:msub><mml:mi mathvariant="normal">obs</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="normal">mod</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:mfenced><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>/</mml:mo><mml:mo>(</mml:mo><mml:mi>n</mml:mi><mml:mo>-</mml:mo><mml:mi>m</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:msqrt><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> of
residuals. Those results are represented in Table 2 for MSR-2 total ozone
datasets inside the vortex and for the three classifications analysed in
this study. Despite trend values after 2001 for the 475 K classification
being
larger by about 28 % than for the 400–600 K classification range, trend
results between both classifications are not significantly different at
2<inline-formula><mml:math id="M156" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> level, suggesting a limited effect of vortex baroclinicity on
trend estimation using MLR analysis. The different results in Table 2
generally present a ratio between trends before and after 2001 close to 3,
similar to that of ODS trends before and after the peak (Chipperfield et
al., 2017). This indicates that the ozone recovery trend could be due to ODS
decrease. Nonetheless this trend cannot be reliably associated with chemical
processes alone and other processes could also play a role.</p>
      <p id="d1e2774">Computed trends over the 2001–2017 September period obtained with our model
range from 1.84 to 2.36 DU yr<inline-formula><mml:math id="M157" 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 all studied cases. They are all
significant at 2<inline-formula><mml:math id="M158" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> level. Solomon et al. (2016) found significant
total ozone trend of 2.5 <inline-formula><mml:math id="M159" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.7 DU yr<inline-formula><mml:math id="M160" 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> in September from SBUV
and ozonesonde observations and similar results from the
Chemistry <inline-formula><mml:math id="M161" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> Dynamics <inline-formula><mml:math id="M162" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> Volcanoes (Chem-Dyn-Vol) simulation
(2.8 <inline-formula><mml:math id="M163" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.6 DU yr<inline-formula><mml:math id="M164" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> using the WACCM.
Estimated total ozone trend when only chemistry is considered in the model
(Chem-Only) correspond to only half of the final trend (1.3 <inline-formula><mml:math id="M165" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1 DU yr<inline-formula><mml:math id="M166" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>.</p>
      <p id="d1e2875">A simulation test was done to evaluate the pertinence of using other proxies
than PWT, HF and GRAD since only these fitted proxies present significant
regression coefficient values at 95 % confidence interval. Results are
represented in Table 2. Slightly lower determination factor <inline-formula><mml:math id="M167" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> is
computed if only PWT, HF and GRAD are considered for September and
comparable residual and trends. This results suggest that the others proxies
provide marginal improvement to the MLR analysis.</p>
</sec>
<sec id="Ch1.S5.SS2.SSS2">
  <title>15 September to 15 October</title>
      <p id="d1e2895">In order to confirm healing of the Antarctic ozone hole, it is important to
evaluate trends for the period where the lowest total ozone values are observed
inside the vortex e.g. between 15 September    and 15 October.
The same analysis as for September is thus performed. Figure 9 illustrates
the results of regression model for total ozone of MSR-2 data series inside
the vortex using the 400–600 K classification. It shows that the
interannual variability of measurements is better represented by the model
than in September. For that period, the determination coefficient <inline-formula><mml:math id="M168" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> is
0.95 (see also Table 3). As for the September regression, the sum of fitted
HF and GRAD proxies (black line in second panel) represents the second
largest contribution to total ozone interannual variability (<inline-formula><mml:math id="M169" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> 13 %
of the total variance) after the PWT proxy (<inline-formula><mml:math id="M170" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> 80 %)
and the last decade of measurement is correctly reproduced by the model.
Significant trends of <inline-formula><mml:math id="M171" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.81 <inline-formula><mml:math id="M172" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.6 DU yr<inline-formula><mml:math id="M173" 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> (<inline-formula><mml:math id="M174" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>29.8 <inline-formula><mml:math id="M175" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3 % decade<inline-formula><mml:math id="M176" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> and
1.42 <inline-formula><mml:math id="M177" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.92 DU yr<inline-formula><mml:math id="M178" 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> (7.3 <inline-formula><mml:math id="M179" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4.7 % decade<inline-formula><mml:math id="M180" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> are estimated before and after 2001. Similar results are
observed if a single level classification is used with larger trend values
after 2001 for 475 K. All trend results are comparable within
<inline-formula><mml:math id="M181" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>2<inline-formula><mml:math id="M182" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>. Results based on the SAT record are similar, with
slightly larger trend values after 2001. Note that the addition in the MLR
analysis of the 2 most recent years (2016–2017), which were characterized by
weak ozone holes, changed the significance of the 2001–2017 trend from
hardly significant to significant better than 2<inline-formula><mml:math id="M183" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>. Results obtained
in the 1980–2017 period by the MLR analysis thus show for the first time a
significant recovery in the 15 September–15 October period. SF, QBO, Antarctic
oscillation and Aer (third panel of Fig. 9) explain <inline-formula><mml:math id="M184" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 % of the
total variance. QBO explains <inline-formula><mml:math id="M185" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>3 DU interannual
variability and Aer signals amount to <inline-formula><mml:math id="M186" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 6 and
<inline-formula><mml:math id="M187" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 3 DU linked to Pinatubo in 1992 and El Chichón in 1983. SF
contribution varies from 4.5 DU during the maximum (except for the last
solar cycle, <inline-formula><mml:math id="M188" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 DU) to <inline-formula><mml:math id="M189" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>2.2 DU during the minimum. AAO
represents negligible contribution. The same test as for September was performed
where proxies of SF, QBO, AAO and Aer were removed from the linear
regression. Results are presented in Table 3. Negligible differences in
trends, <inline-formula><mml:math id="M190" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> and residuals are observed depending on whether those proxies are considered
in the MLR analysis. In addition, lower <inline-formula><mml:math id="M191" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula> values are found
for smaller number of fitted parameters, which is the case for the
regression using PWT, HF and GRAD only.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9"><caption><p id="d1e3106">As in Fig. 8 but for 15 September–15 October.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f09.png"/>

          </fig>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T3" specific-use="star"><caption><p id="d1e3118">Same as Table 2 but for 15 September–15 October period. SAT dataset is also
presented.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="7">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry namest="col2" nameend="col4" align="center">Multi-sensor reanalysis (MSR-2) </oasis:entry>
         <oasis:entry namest="col5" nameend="col7" align="center">Composite satellite data (SAT) </oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">400–600 K</oasis:entry>
         <oasis:entry colname="col3">475 K</oasis:entry>
         <oasis:entry colname="col4">550 K</oasis:entry>
         <oasis:entry colname="col5">400–600 K</oasis:entry>
         <oasis:entry colname="col6">475 K</oasis:entry>
         <oasis:entry colname="col7">550 K</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M192" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.95</oasis:entry>
         <oasis:entry colname="col3">0.94</oasis:entry>
         <oasis:entry colname="col4">0.94</oasis:entry>
         <oasis:entry colname="col5">0.96</oasis:entry>
         <oasis:entry colname="col6">0.94</oasis:entry>
         <oasis:entry colname="col7">0.94</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend before 2001</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M193" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.81 <inline-formula><mml:math id="M194" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.60</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M195" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.55 <inline-formula><mml:math id="M196" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.66</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M197" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.63 <inline-formula><mml:math id="M198" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.77</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M199" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.86 <inline-formula><mml:math id="M200" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.57</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M201" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.57 <inline-formula><mml:math id="M202" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.64</oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M203" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.64 <inline-formula><mml:math id="M204" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.65</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend after 2001</oasis:entry>
         <oasis:entry colname="col2">1.42 <inline-formula><mml:math id="M205" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.92</oasis:entry>
         <oasis:entry colname="col3">1.73 <inline-formula><mml:math id="M206" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.01</oasis:entry>
         <oasis:entry colname="col4">1.58 <inline-formula><mml:math id="M207" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.02</oasis:entry>
         <oasis:entry colname="col5">1.70 <inline-formula><mml:math id="M208" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.87</oasis:entry>
         <oasis:entry colname="col6">1.96 <inline-formula><mml:math id="M209" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.99</oasis:entry>
         <oasis:entry colname="col7">1.79 <inline-formula><mml:math id="M210" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.99</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"><inline-formula><mml:math id="M211" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">9.67</oasis:entry>
         <oasis:entry colname="col3">10.65</oasis:entry>
         <oasis:entry colname="col4">10.77</oasis:entry>
         <oasis:entry colname="col5">9.21</oasis:entry>
         <oasis:entry colname="col6">10.39</oasis:entry>
         <oasis:entry colname="col7">10.46</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry namest="col2" nameend="col7" align="center">Only with GRAD, HF and PWT </oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M212" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.94</oasis:entry>
         <oasis:entry colname="col3">0.93</oasis:entry>
         <oasis:entry colname="col4">0.93</oasis:entry>
         <oasis:entry colname="col5">0.95</oasis:entry>
         <oasis:entry colname="col6">0.93</oasis:entry>
         <oasis:entry colname="col7">0.93</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend before 2001</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M213" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.86 <inline-formula><mml:math id="M214" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.56</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M215" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.71 <inline-formula><mml:math id="M216" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.64</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M217" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.67 <inline-formula><mml:math id="M218" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.64</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M219" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.93 <inline-formula><mml:math id="M220" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.56</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M221" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.75 <inline-formula><mml:math id="M222" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.66</oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M223" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.70 <inline-formula><mml:math id="M224" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.63</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend after 2001</oasis:entry>
         <oasis:entry colname="col2">1.21 <inline-formula><mml:math id="M225" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.83</oasis:entry>
         <oasis:entry colname="col3">1.42 <inline-formula><mml:math id="M226" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.95</oasis:entry>
         <oasis:entry colname="col4">1.35 <inline-formula><mml:math id="M227" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.94</oasis:entry>
         <oasis:entry colname="col5">1.40 <inline-formula><mml:math id="M228" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.83</oasis:entry>
         <oasis:entry colname="col6">1.56 <inline-formula><mml:math id="M229" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.97</oasis:entry>
         <oasis:entry colname="col7">1.47 <inline-formula><mml:math id="M230" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.93</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"><inline-formula><mml:math id="M231" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">9.35</oasis:entry>
         <oasis:entry colname="col3">10.68</oasis:entry>
         <oasis:entry colname="col4">10.65</oasis:entry>
         <oasis:entry colname="col5">9.35</oasis:entry>
         <oasis:entry colname="col6">10.84</oasis:entry>
         <oasis:entry colname="col7">10.55</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry namest="col2" nameend="col7" align="center">Only with HF and PWT </oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M232" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.87</oasis:entry>
         <oasis:entry colname="col3">0.82</oasis:entry>
         <oasis:entry colname="col4">0.86</oasis:entry>
         <oasis:entry colname="col5">0.88</oasis:entry>
         <oasis:entry colname="col6">0.83</oasis:entry>
         <oasis:entry colname="col7">0.87</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend before 2001</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M233" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.89 <inline-formula><mml:math id="M234" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.84</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M235" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.74 <inline-formula><mml:math id="M236" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.98</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M237" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.70 <inline-formula><mml:math id="M238" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.86</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M239" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.96 <inline-formula><mml:math id="M240" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.82</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M241" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.78 <inline-formula><mml:math id="M242" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.00</oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M243" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5.72 <inline-formula><mml:math id="M244" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.84</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend after 2001</oasis:entry>
         <oasis:entry colname="col2">1.45 <inline-formula><mml:math id="M245" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.24</oasis:entry>
         <oasis:entry colname="col3">1.70 <inline-formula><mml:math id="M246" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.45</oasis:entry>
         <oasis:entry colname="col4">1.57 <inline-formula><mml:math id="M247" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.27</oasis:entry>
         <oasis:entry colname="col5">1.63 <inline-formula><mml:math id="M248" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.21</oasis:entry>
         <oasis:entry colname="col6">1.82 <inline-formula><mml:math id="M249" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.47</oasis:entry>
         <oasis:entry colname="col7">1.68 <inline-formula><mml:math id="M250" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.24</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M251" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">14.06</oasis:entry>
         <oasis:entry colname="col3">16.40</oasis:entry>
         <oasis:entry colname="col4">14.39</oasis:entry>
         <oasis:entry colname="col5">13.71</oasis:entry>
         <oasis:entry colname="col6">16.18</oasis:entry>
         <oasis:entry colname="col7">14.03</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <?pagebreak page7566?><p id="d1e3903">The different cases shown in Table 3 present significant trends at 2<inline-formula><mml:math id="M252" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> over the 1980–2000 and the 2001–2017 periods. The computed trend with 400–600 K
range classification is comparable to the Chem-Only trend calculated
by WACCM in Solomon et al. (2016). Despite the good agreement between
regressed values and measurements, especially for the period of 15 September–15 October and
for the range classification method (400–600 K), it is not possible to
attribute ozone significant increase to ODS decrease. In addition, the ratio
between trends before and after 2001 is larger than 3, which could be
due to the effect of desaturation of the ozone loss.</p>
</sec>
<sec id="Ch1.S5.SS2.SSS3">
  <title>Impact of GRAD proxy on trend estimation</title>
      <p id="d1e3919">The HF proxy represents the cumulative effect of wave activity on vortex
stability (e.g. a high HF corresponds to a warmer vortex) that seems
insufficient to represent total ozone variability over the last decade,
especially in 2010 and 2012. The GRAD proxy was developed in order to
also consider  the vortex stability during both studied periods. Since
Aer, QBO, SF and AAO represent lower contribution to ozone variability,
trend analyses using HF, PWT proxies only and including (or not) the GRAD
proxy are performed in order to highlight the impact of this parameter.
Figure 10 shows residuals of MLR analysis with and without GRAD on MSR-2
data inside the vortex for the 400–600 K classification range for
September and 15 September–15 October periods. The residual anomalies are significantly
reduced after 2002 when GRAD is used, especially in the 15 September–15 October period.
The second panels of Figs. 8 and 9 show that in some years HF and GRAD
proxies are in phase, as during 2009–2014 when GRAD intensifies the HF
contribution to ozone variability. This improvement is especially visible
for the years 2010 and 2012. When both proxies are anticorrelated, as in
2005–2008, the improvement linked to the GRAD proxy is also observed. Tables 2 and 3
show the results of the regressions excluding GRAD proxy for
September and 15 September–15 October, respectively. The determination
coefficient is generally reduced by <inline-formula><mml:math id="M253" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 0.07 and the <inline-formula><mml:math id="M254" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula>
values are 25  to 50 % larger. Trend values are mostly similar but
the error bars are reduced when GRAD is used as explanatory variable,
especially after 2001. Trends over the 2001–2017 period estimated without
the GRAD proxy are still significant at 2<inline-formula><mml:math id="M255" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> in September and
15 September–15 October for both datasets.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F10"><caption><p id="d1e3945">Residual (in DU) with and without contribution of GRAD proxy for
September <bold>(a)</bold> and 15 September–15 October period <bold>(b)</bold>.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f10.png"/>

          </fig>

</sec>
<?pagebreak page7567?><sec id="Ch1.S5.SS2.SSS4">
  <title>PWT vs. PWLT</title>
      <p id="d1e3967">In order to evaluate the improvement of an additional parabolic function to
the linear functions of the piece-wise trend proxy, the classical PWLT is applied in the MLR analysis of MSR-2 datasets.
Figure S1 in the Supplement shows average total ozone anomalies of MSR-2 inside the vortex
(400–600 K range classification method) in September and 15 September–15 October and
the retrieved trends using both the PWLT and PWT methods. In the case of the
15 September–15 October period, the PWT model provides a better representation of
long-term ozone evolution compared to PWLT, as it better captures ozone loss
saturation during the 1990s. The trend error bars are also smaller using
PWT before and after 2001. In addition, a better agreement between
measurements and model values is observed with a larger <inline-formula><mml:math id="M256" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> and lower
residuals. The 2001–2017 trend error bars are <inline-formula><mml:math id="M257" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 60 % larger
when PWLT is used and the trend value itself is nearly double. In the case of
September, a slight improvement in <inline-formula><mml:math id="M258" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>, residuals and error bars is
obtained with PWT. The 2001–2017 trend value with PWLT is 40 % larger.</p>
</sec>
</sec>
<sec id="Ch1.S5.SS3">
  <title>Results using OMD metric</title>
      <p id="d1e4006">OMD has been used in previous studies to evaluate ozone loss and ozone
recovery (e.g. de Laat et al., 2017). This metric has the advantage to be
independent of the vortex position. Total ozone MSR-2 data were used to
compute the average daily OMD on September and 15 September–15 October
periods. The total ozone columns are referenced to the 220 DU threshold
value and the corresponding mass deficit of the partial column (220 DU –
total ozone column) is computed at each grid point (e.g. Bodeker and
Scourfield, 1995). Only total ozone columns south of 60<inline-formula><mml:math id="M259" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and lower
than 220 DU are considered and the daily OMDs correspond to the sum of OMD
at each pixel multiplied by the cosine of the latitude and the square of the
Earth's radius. Table 4 shows the MLR analysis of OMD using different sets of
proxies as for ozone average in Tables 2 and 3. The contributions of Aer,
AAO, QBO and SF do not shown an impact on MLR analysis, where similar
<inline-formula><mml:math id="M260" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M261" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula>, trend and error bars values are obtained. However, the
inclusion of GRAD results in larger <inline-formula><mml:math id="M262" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> and lower residuals in both
periods. For the different cases and periods shown in Table 4, the OMD trend
values are significant at 2<inline-formula><mml:math id="M263" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>. The MLR analysis using GRAD, HF and PWT
proxies provides trends before and after 2001 of
<inline-formula><mml:math id="M264" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.29 <inline-formula><mml:math id="M265" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.24 and 0.86 <inline-formula><mml:math id="M266" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.36 Mt yr<inline-formula><mml:math id="M267" 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> in September and
<inline-formula><mml:math id="M268" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.61 <inline-formula><mml:math id="M269" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.22 and 0.65 <inline-formula><mml:math id="M270" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.33 Mt yr<inline-formula><mml:math id="M271" 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> in
15 September–15 October. De Laat el al. (2017) found a similar trend for the
recovery period of 0.77 Mt yr<inline-formula><mml:math id="M272" 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 the averaged OMD between days 220
and 280 of the year. Figure 11 displays the comparison between the OMD
records and results of MLR analysis for the September and
15 September–15 October period, together with the trend components of the
model. The effect of ozone loss saturation is particularly visible in the
15 September–15 October period. There are some years that are not totally
explained by the model, e.g. 2002 and 2004 for both periods and 2000 for
September. The contributions of GRAD, HF and GRAD <inline-formula><mml:math id="M273" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> HF are shown in upper
panels of Fig. S2, where GRAD intensifies HF contribution in 2010 and 2012,
while both proxies are anticorrelated in 2005–2008 as observed for the total
ozone analysis. The residuals with and without GRAD are shown in the bottom
panels of Fig. S2. The improvement linked to the use of GRAD proxy is
particularly visible in the last decade.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F11"><caption><p id="d1e4143">OMD (in Mt) computed from total columns of MSR-2 dataset lower than
220 DU and south of 60<inline-formula><mml:math id="M274" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S for September <bold>(a)</bold> and 15 September–15 October <bold>(b)</bold>.
Regressed values by MLR analysis using GRAD, HF and PWT are
also shown as well as the fitted PWT proxy.</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f11.png"/>

        </fig>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T4"><caption><p id="d1e4170">Coefficient of determination <inline-formula><mml:math id="M275" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> and trends <inline-formula><mml:math id="M276" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>2<inline-formula><mml:math id="M277" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> in
Mt yr<inline-formula><mml:math id="M278" 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> before and after the turnaround year 2001 derived from
multi-regression model using OMD dataset (MSR-2 total ozone columns and
threshold of 220 DU; see the text) for September and 15 September–15 October over
1980–2017 period. The residual is represented in Mt by <inline-formula><mml:math id="M279" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula> as
explained in Table 2.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="3">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">September</oasis:entry>
         <oasis:entry colname="col3">15 Sep–15 Oct</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M280" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.85</oasis:entry>
         <oasis:entry colname="col3">0.91</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend before 2001</oasis:entry>
         <oasis:entry colname="col2">1.28 <inline-formula><mml:math id="M281" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.25</oasis:entry>
         <oasis:entry colname="col3">1.59 <inline-formula><mml:math id="M282" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.24</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend after 2001</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M283" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.78 <inline-formula><mml:math id="M284" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.39</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M285" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.68 <inline-formula><mml:math id="M286" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.37</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"><inline-formula><mml:math id="M287" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">4.04</oasis:entry>
         <oasis:entry colname="col3">3.85</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry namest="col2" nameend="col3" align="center">Only GRAD, HF and PWT </oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M288" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.82</oasis:entry>
         <oasis:entry colname="col3">0.90</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend before 2001</oasis:entry>
         <oasis:entry colname="col2">1.29 <inline-formula><mml:math id="M289" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.24</oasis:entry>
         <oasis:entry colname="col3">1.61 <inline-formula><mml:math id="M290" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.22</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend after 2001</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M291" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.86 <inline-formula><mml:math id="M292" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.36</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M293" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.65 <inline-formula><mml:math id="M294" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.33</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"><inline-formula><mml:math id="M295" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">4.04</oasis:entry>
         <oasis:entry colname="col3">3.68</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry namest="col2" nameend="col3" align="center">Only HF and PWT </oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M296" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.78</oasis:entry>
         <oasis:entry colname="col3">0.85</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend before 2001</oasis:entry>
         <oasis:entry colname="col2">1.29 <inline-formula><mml:math id="M297" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.26</oasis:entry>
         <oasis:entry colname="col3">1.61 <inline-formula><mml:math id="M298" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.27</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Trend after 2001</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M299" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.88 <inline-formula><mml:math id="M300" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.38</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M301" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.70 <inline-formula><mml:math id="M302" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.39</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M303" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">4.37</oasis:entry>
         <oasis:entry colname="col3">4.44</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d1e4570">As for total ozone, MLR analysis using PWLT was performed for comparison
with the PWT model. Figure S3 shows the OMD records together with PWLT and
PWT components of the regression model for the both periods. Similar
agreement is obtained for September but the regression results in larger
residuals for 15 September–15 October using PWLT (not shown). A major difference is
observed in the period 2001–2017, with a large trend value of <inline-formula><mml:math id="M304" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.91 <inline-formula><mml:math id="M305" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.41 Mt yr<inline-formula><mml:math id="M306" 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>,
corresponding to an increase of 40 % in absolute
value.</p><?xmltex \hack{\newpage}?>
</sec>
</sec>
<?pagebreak page7568?><sec id="Ch1.S6">
  <title>Temporal evolution of low total ozone values inside the vortex</title>
      <p id="d1e4607">The ozone hole is generally defined as the region with total ozone columns
lower than 220 DU. This standard value was used in different studies to
evaluate the ozone depletion from the OHA (e.g. Newman et
al., 2006; Solomon et al., 2016) or the OMD (e.g. de
Laat and van Weele, 2011; de Laat et al., 2017) metrics. In order to
evaluate how the ozone hole is influenced by very low ozone values, the
surface relative to the vortex area occupied by ozone values lower than
different threshold levels is computed for each day and averaged over
different periods (September, 15 September–15 October and October). The top panel of
Fig. 12 shows the evolution of these average relative areas for five
different thresholds: 220, 200, 175, 150 and 125 DU for the
15 September–15 October period. MSR-2 datasets are used for this analysis and vortex
areas are estimated using the 400–600 K range classification, the results
of previous sections having shown that the range classification better
constrains the OHA. Results show increasing areas during the
1980s, a stabilization in the 1990s and a larger interannual variability
since 2001. In contrast to the 220 DU threshold case, the evolution of
relative areas corresponding to lower thresholds shows a delayed increase
from the beginning of the 1980s to the early 1990s, reaching a maximum in all
cases in 2000. After 2000, a larger interannual variability is generally
observed and from 2006 a steady decrease is seen for thresholds lower than
200 DU. In all cases, several anomalous years are observed with important
reduction of ozone depletion: 1988, 1991, 2002, 2004, 2010 and 2012. Note
that these years correspond to a high contribution of HF and GRAD proxies to
the regressed ozone values (Fig. 9, second panel). If we exclude these
anomalous years, the 220 DU relative area remains fairly stable at about
90 % of the total vortex in average since 1990. In the most recent years,
relative areas for 125 and 150 DU thresholds decrease to less than 10
and 30 %, respectively, from their peak value of 21  and 57 %
reached in 2000. If such trend persists, the frequency of very low ozone
values (e.g. below 125 DU) is expected to become negligible in the coming
decade.</p>
      <p id="d1e4610">In addition, OMD were computed for the same thresholds (bottom panel of Fig. 12).
The evolutions of OMD present similar behaviour as the relative area,
but in this case OMD at 220 DU threshold shows a visible decrease since
2000. Nowadays OMD at a threshold lower than 150 DU presents very small values
lower than 0.2 Mt.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F12"><caption><p id="d1e4615">Relative area inside the vortex (in percent) with values lower than
five level thresholds (125, 150, 175, 200 and 220 DU) computed from MSR-2
dataset using 400–600 K classification on 15 September–15 October period <bold>(a)</bold>.
OMD (in Mt) time series computed from MSR-2 total ozone data for the same
five
thresholds and time period are displayed in panel <bold>(b)</bold>.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f12.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F13"><caption><p id="d1e4633">Start day of occurrences of total ozone levels lower than
different thresholds (125, 150, 175, 200 and 220 DU) computed from the MSR-2
dataset using the 400–600 K classification between 1 September   and
15 October.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7557/2018/acp-18-7557-2018-f13.png"/>

      </fig>

      <?pagebreak page7569?><p id="d1e4642">Solomon et al. (2016) have highlighted for the first time a delay in the
formation of the ozone hole after 2000. This shift can be explained by the
slower ozone loss rates after sun appearance over the pole due to ODS
decrease in the polar stratosphere. In this work, such a time shift
was investigated by computing the first day when ozone levels below certain
thresholds occur inside the vortex (using the 400–600 K classification
range), from 1 September   to 15 October   (Fig. 13). The same
thresholds values as for Fig. 12 were used. In order to avoid influence of
spurious values, the number of 1<inline-formula><mml:math id="M307" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M308" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1<inline-formula><mml:math id="M309" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> grid cells
with total ozone columns below the various thresholds in the first day (or
start day) has to be larger than 10. For each curve, day values equal to
<inline-formula><mml:math id="M310" display="inline"><mml:mrow><mml:mn mathvariant="normal">244</mml:mn><mml:mo>/</mml:mo><mml:mn mathvariant="normal">245</mml:mn></mml:mrow></mml:math></inline-formula> correspond to years when ozone levels below the corresponding
threshold have appeared at or before the beginning of September. For the 220 DU
threshold, the dark blue curve shows that this is the case since 1983. For
the 200 DU threshold, lower ozone values appear before the beginning of
September after the mid-1980s. For the other thresholds, we observe a
decrease, with some variability, of the start day during the 1980s, the two lowest thresholds in  the
1990s and an increase after 2000–2005. This
increase is most visible on the 125 DU threshold curve and to some extent
also on the 150 DU threshold curve. In 2016, ozone levels below 150 DU have
appeared in the beginning of September, similar to ozone holes at the
end of the 1990s, but levels below 125 DU still appeared later. No values for a
particular year in the threshold curves indicate that total ozone levels were
above that threshold during the whole period considered. This is the case for
the two lower thresholds before 1985 and for the 125 DU threshold in 2002,
2004 and 2017.</p>
</sec>
<sec id="Ch1.S7" sec-type="conclusions">
  <title>Conclusions</title>
      <p id="d1e4688">MSR-2 and SAT (TOMS and OMI with gaps in 1993–1995 filled by MSR-2) datasets
have been used to evaluate total ozone trends within the southern polar
vortex over the 1980–2017 period. A multi-regression model is applied to
ozone values averaged over the month of September  and the 15 September to 15
October period in order to compute long-term trends before and after the ODS
peak in the polar stratosphere that occurred around 2001 (Newman et al.,
2007). The 15 September–15 October time range corresponds to the period of
maximum ozone depletion. It was not commonly used in previous works. Proxies
and time windows for averaging them are selected following de Laat et al. (2015) work.</p>
      <p id="d1e4691">For the classification of total ozone measurements inside the vortex, the
classical Nash et al. (1996) method is used. In order to evaluate the impact
of vortex baroclinicity on trend analysis, classifications using a single
isentropic levels (475 and 550 K) and
a range of levels (400–600 K) are
tested. Systematic differences are found between the various datasets. However, the
interannual variability is similar, with correlation coefficients ranging
from 0.98 to 0.99 in both studied periods. While larger trend values are
generally found with the 475 K classification, the differences with trends
related to the 400–600 K range classification are not significant at
2<inline-formula><mml:math id="M311" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> level.</p>
      <p id="d1e4701">The use of combined piece-wise linear and parabolic functions for the trend
proxies (PWT) in the 1980–2000 and 2001–2017 periods provides a good
representation of the total ozone long-term behaviour inside the vortex
(after removal of interannual variability), especially for the 15 September–15 October
period, probably in relation to the effect of ozone loss saturation. The
classical PWLT used in previous studies seems to overestimate the trends
during the recovery period.</p>
      <p id="d1e4704">A new proxy (GRAD) representing the vortex stability over both studied
periods is included in the multilinear regression. This proxy improves the
representation of total ozone interannual variability by the regressed
values especially over the last decade. It results in a <inline-formula><mml:math id="M312" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 0.05
larger value for the <inline-formula><mml:math id="M313" display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> determination coefficient, lower fitted
residuals and smaller trend uncertainties for the different classification
methods and datasets. In general, the best agreement between observations
and regressed values is found for the 15 September–15 October period. While the HF
combined with GRAD proxies reproduce the interannual variability
of ozone quite well, other proxies such as Aer, QBO, SF and AAO present smaller
explanatory power and contribute less to reduce trend uncertainties.</p>
      <p id="d1e4726">In the period of increasing ODSs (1980–2000), the MLR analysis shows negative
and significant trends for both studied periods, similar to values found in
previous studies (e.g. Kuttippurath et al., 2013, and de Laat et al., 2015).
The 15 September–15 October period presents slightly larger negative trends in absolute
value than the month of September.</p>
      <p id="d1e4729">In the 2001–2017 period, positive trends are obtained for all scenarios. The
largest trends and highest significance are found for the September period,
with a trend value of 1.84 <inline-formula><mml:math id="M314" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1 DU for the MSR-2 total ozone record
using the 400–600 K range classification method. For the 15 September–15 October
period, a lower trend of 1.42 <inline-formula><mml:math id="M315" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.92 DU is obtained using the same
record. Better fit and smaller residuals are obtained for that period.
Differences with trend results from the other SAT dataset evaluated in the
study are not statistically significant.</p>
      <p id="d1e4746">The ratio between trends before and after 2001 varies according to the
studied period. Only September trends present a ratio of <inline-formula><mml:math id="M316" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 3
as expected for an ozone response to ODS evolution. However, as for other
trend studies based on MLR fit to observations, it is not possible from this
analysis alone to fully attribute the retrieved trends to ODS evolution. For
such a study, a combination of model and observations is needed. Potential
feedbacks between chemistry, radiation and dynamics will play a role in
ozone recovery. A recent study indicates an increase in temperatures within
the vortex core from MERRA reanalyses during the period 2000–2014<?pagebreak page7570?> in
austral spring and summer (Solomon et al., 2017). Such a temperature
increase that could be linked to ozone increase could play a role in the
decrease of occurrence of low ozone values within the vortex and subsequent
ozone increase.</p>
      <p id="d1e4756">The evolution of OMD was also analysed using MSR-2 data. MLR
analysis on this metric confirms the findings obtained for total ozone
columns, e.g. a general improvement of the fits with the GRAD proxy and the
main explanatory power provided by the GRAD, HF and PWT proxies. The
2001–2017 OMD trends are larger in absolute value for September
(<inline-formula><mml:math id="M317" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.86 <inline-formula><mml:math id="M318" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.36 Mt yr<inline-formula><mml:math id="M319" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> than for 15 September–15 October (<inline-formula><mml:math id="M320" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.65 <inline-formula><mml:math id="M321" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.33 Mt yr<inline-formula><mml:math id="M322" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>.
They are significant at 2<inline-formula><mml:math id="M323" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> level in both cases. These
results are in general good agreement with those obtained in de Laat et al. (2017). Similar reductions
of 53 and 35 % of OMD are computed for
September and 15 September–15 October, respectively. This is consistent with the
30–40 % change in ODSs relative to their level in 1980, when total ozone
values below the 220 DU threshold started to appear systematically (WMO,
2011).</p>
      <p id="d1e4825">The structural uncertainties of the MLR analysis linked to the selection of
proxies were not fully analysed in this work, as in de Laat et al. (2015).
The main sensitivity tests concerned the baroclinicity of the vortex and the
impact of its stability during the studied periods. Trend differences in the
various scenarios analysed provide some quantification of related
uncertainties and are lower than the statistical trend uncertainties.
Further, the large determination coefficients obtained for both periods
analysed give confidence in the retrieved trends. The heat flux proxy that
provides the largest explanatory power in the various fits is a well-known
driver of vortex temperature conditions that are the primary causes of polar
ozone depletion in periods of high ODS levels. The influence of the GRAD
proxy in recent years highlights the importance of the vortex stability for
the containment of the ozone hole during the period of maximum depletion.</p>
      <p id="d1e4828">Polar ozone recovery was also evaluated by examining the temporal evolution
of relative areas occupied by ozone levels below various thresholds within
the vortex. Very small total ozone columns (&lt; 150 DU) did not occur
inside the vortex before the late 1980s and early 1990s. For the 125, 150
and 175 DU thresholds, relative areas display a steady decrease since the
beginning of the 21st  century, while for the 200 and 220 DU
thresholds, the relative area's evolution is quite stable. All relative area
curves are marked by increased variability since 2000. Relative areas
related to the lowest thresholds show a more rapid decrease, which further
points towards polar ozone recovery. OMD records based on the same
thresholds show a similar behaviour.</p>
      <p id="d1e4832">In summary, this work present clear symptoms of polar ozone recovery.
Recovery is found for the month of September and for the first time for the
period of maximum ozone depletion, e.g. from 15 September  to 15 October. For
both studied periods, recovery is deduced from the significant positive
trends in total ozone, significant negative trends of ozone mass deficit and
from the steady decrease of the occurrence of low ozone values within the
polar vortex. As ODSs continue to decrease in the next years, it is likely
that ozone recovery in the polar vortex in spring will become more evident.</p>
</sec>

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

      <p id="d1e4839">The satellite data used to build the aerosol
proxy were created by Sergey Khaykin and are available at
<uri>https://drive.google.com/open?id=1lql_p0xuPpVcWVnSJhVWW6FVPTFz3ift</uri>,
last access: 28 May 2018.</p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d1e4845">The supplement related to this article is available online at: <inline-supplementary-material xlink:href="https://doi.org/10.5194/acp-18-7557-2018-supplement" xlink:title="pdf">https://doi.org/10.5194/acp-18-7557-2018-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="competinginterests">

      <p id="d1e4854">The authors declare that they have no conflict of interest.</p>
  </notes><notes notes-type="sistatement">

      <p id="d1e4860">This article is part of the special issue “Quadrennial Ozone
Symposium 2016 – Status and trends of atmospheric ozone (ACP/AMT
inter-journal SI)”. It is a result of the Quadrennial Ozone Symposium 2016,
Edinburgh, United Kingdom, 4–9 September 2016.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e4866">The authors thank NASA's GSFC and TEMIS for total ozone column data of
TOMS/SBUV/OMI-TOMS and MSR-2, respectively. They are grateful to Cathy Boone
of ESPRI data centre of Institut Pierre Simone Laplace (IPSL) for providing ERA-Interim data.
This work was supported by the Dynozpol/LEFE project funded by
the French Institut National des Sciences de l'Univers (INSU) of the Centre
National de la Recherche Scientifique (CNRS). The authors thank Susan Solomon
for fruitful interactions and the two anonymous referees
for their constructive reviews.<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>
Edited by:  Richard Eckman  <?xmltex \hack{\newline}?>
Reviewed by:  two anonymous referees</p></ack><ref-list>
    <title>References</title>

      <ref id="bib1.bib1"><label>1</label><mixed-citation>Allen, D., Bevilacqua, R., Nedoluha, G., Randall, C., and Manney, G.:
Unusual stratospheric transport and mixing during 2002 Antarctic winter,
Geophys. Res. Lett., 30, 1599, <ext-link xlink:href="https://doi.org/10.1029/2003GL017117" ext-link-type="DOI">10.1029/2003GL017117</ext-link>, 2003.</mixed-citation></ref>
      <ref id="bib1.bib2"><label>2</label><mixed-citation>
Bhartia, P. K. and Wellemeyer, C.: TOMS-V8 total O3 algorithm, in OMI
Algorithm Theoretical Basis Document, vol. II, OMI Ozone Products, edited
by: P. K. Bhartia,  15–31, NASA Goddard Space Flight Center, Greenbelt,
Maryland, USA, 2002.</mixed-citation></ref>
      <ref id="bib1.bib3"><label>3</label><mixed-citation>
Bodeker, G. E. and Scourfield, M. W. J.: Planetary waves in total ozone and
their relation to Antarctic ozone depletion, Geophys. Res. Lett., 22,
2949–2952, 1995.</mixed-citation></ref>
      <?pagebreak page7571?><ref id="bib1.bib4"><label>4</label><mixed-citation>Bodeker, G. E., Struthers, H., and Connor, B. J.: Dynamical containment of
Antarctic ozone depletion, Geophys. Res. Lett., 29, 1098,
<ext-link xlink:href="https://doi.org/10.1029/2001GL014206" ext-link-type="DOI">10.1029/2001GL014206</ext-link>, 2002.</mixed-citation></ref>
      <ref id="bib1.bib5"><label>5</label><mixed-citation>Chipperfield, M., Bekki, S., Dhomse, S., Harris, N. R. P., Hassler, B.,
Hossaini, R., Steinbrecht, W., Thiéblemont, R., and Weber, M.: Detecting
recovery of stratospheric ozone layer, Nature, 549, 211–218,
<ext-link xlink:href="https://doi.org/10.1038/nature23681" ext-link-type="DOI">10.1038/nature23681</ext-link>, 2017.</mixed-citation></ref>
      <ref id="bib1.bib6"><label>6</label><mixed-citation>Chubachi, S.: A special observation at Syowa station, Antarctica from
February 1982 to January 1983, in: Atmospheric Ozone, edited by: Zerefos, C.
and A. Ghazi, Springer, the Netherlands, 285–289,
<ext-link xlink:href="https://doi.org/10.1007/978-94-009-5313-0_58" ext-link-type="DOI">10.1007/978-94-009-5313-0_58</ext-link>, 1985.</mixed-citation></ref>
      <ref id="bib1.bib7"><label>7</label><mixed-citation>Farman, J. C., Gardiner, B. G., and Shanklin, J. D.: Large losses of total
ozone in Antarctica reveal seasonal ClOx/NOx interaction, Nature, 315,
207–210, <ext-link xlink:href="https://doi.org/10.1038/315207a0" ext-link-type="DOI">10.1038/315207a0</ext-link>, 1985.</mixed-citation></ref>
      <ref id="bib1.bib8"><label>8</label><mixed-citation>Dee, D. P., Uppala, S. M., Simmons, A. J., Berrisford, P., Poli, P.,
Kobayashi, S., Andrae, U., Balmaseda, M. A., Balsamo, G., Bauer, P.,
Bechtold, P., Beljaars, A. C. M., van de Berg, L., Bidlot, J., Bormann, N.,
Delsol, C., Dragani, R., Fuentes, M., Geer, A. J., Haimberger, L., Healy, S.
B., Hersbach, H., Hólm, E. V., Isaksen, L., Kållberg, P., Köhler,
M., Matricardi, M., McNally, A. P., Monge-Sanz, B. M., Morcrette, J.-J.,
Park, B.-K., Peubey, C., de Rosnay, P., Tavolato, C., Thépaut, J.-N., and
Vitart, F.: The ERA-Interim reanalysis: configuration and performance of the
data assimilation system, Q. J. R. Meteorol. Soc., 137, 553–597,
<ext-link xlink:href="https://doi.org/10.1002/qj.828" ext-link-type="DOI">10.1002/qj.828</ext-link>, 2011.</mixed-citation></ref>
      <ref id="bib1.bib9"><label>9</label><mixed-citation>de Laat, A. T. J. and van Weele, M.: The 2010 Antarctic ozone hole: Observed
reduction in ozone destruction by minor sudden stratospheric warmings, Sci.
Rep., 1, 38,
<ext-link xlink:href="https://doi.org/10.1038/srep00038" ext-link-type="DOI">10.1038/srep00038</ext-link>, 2011.</mixed-citation></ref>
      <ref id="bib1.bib10"><label>10</label><mixed-citation>de Laat, A. T. J., van der A, R. J., and van Weele, M.: Tracing the second
stage of ozone recovery in the Antarctic ozone-hole with a “big data”
approach to multivariate regressions, Atmos. Chem. Phys., 15, 79–97,
<ext-link xlink:href="https://doi.org/10.5194/acp-15-79-2015" ext-link-type="DOI">10.5194/acp-15-79-2015</ext-link>, 2015.</mixed-citation></ref>
      <ref id="bib1.bib11"><label>11</label><mixed-citation>de Laat, A. T. J., van Weele, M., and van der A, R. J.: Onset of
Stratospheric Ozone Recovery in the Antarctic Ozone Hole in Assimilated
Daily Total Ozone Columns, J. Geophys. Res., 122, 11880–11899,
<ext-link xlink:href="https://doi.org/10.1002/2016JD025723" ext-link-type="DOI">10.1002/2016JD025723</ext-link>,   2017.</mixed-citation></ref>
      <ref id="bib1.bib12"><label>12</label><mixed-citation>Godin, S., Bergeret, V., Bekki, S., David, C., and Mégie, G.: Study of
the interannual ozone loss and the permeability of the Antarctic polar vortex
from aerosols and ozone lidar measurements in Dumont d'Urville
(66.4<inline-formula><mml:math id="M324" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S, 140<inline-formula><mml:math id="M325" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E), J. Geophys. Res., 106, 1311–1330,
<ext-link xlink:href="https://doi.org/10.1029/2000JD900459" ext-link-type="DOI">10.1029/2000JD900459</ext-link>, 2001.</mixed-citation></ref>
      <ref id="bib1.bib13"><label>13</label><mixed-citation>Hauchecorne, A., Chanin, M.-L., and Keckhut, P.: Climatology and trends of
the middle atmospheric temperature (33–87 km) as seen by Rayleigh lidar
over the south of France, J. Geophys. Res., 96, 15297–15309,
<ext-link xlink:href="https://doi.org/10.1029/91JD01213" ext-link-type="DOI">10.1029/91JD01213</ext-link>, 1991.</mixed-citation></ref>
      <ref id="bib1.bib14"><label>14</label><mixed-citation>Hauchecorne, A., Godin, S., Marchand, M., Heese, B., and Souprayen, C.:
Estimation of the Transport of Chemical Constituents from the Polar Vortex to
Middle Latitudes in the Lower Stratosphere using the High-Resolution
Advection Model MIMOSA and Effective Diffusivity, J. Geophys. Res., 107,
8289, <ext-link xlink:href="https://doi.org/10.1029/2001JD000491" ext-link-type="DOI">10.1029/2001JD000491</ext-link>, 2002.</mixed-citation></ref>
      <ref id="bib1.bib15"><label>15</label><mixed-citation>Kerzenmacher, T. E., Keckhut, P., Hauchecorne, A., and Chanin, M.-L.:
Methodological uncertainties in multi-regression analyses of
middle-atmospheric data series, J. Environ. Monitor., 7, 682–690,
<ext-link xlink:href="https://doi.org/10.1039/B603750J" ext-link-type="DOI">10.1039/B603750J</ext-link>, 2006.</mixed-citation></ref>
      <ref id="bib1.bib16"><label>16</label><mixed-citation>Khaykin, S. M., Godin-Beekmann, S., Keckhut, P., Hauchecorne, A., Jumelet,
J., Vernier, J.-P., Bourassa, A., Degenstein, D. A., Rieger, L. A., Bingen,
C., Vanhellemont, F., Robert, C., DeLand, M., and Bhartia, P. K.: Variability
and evolution of the midlatitude stratospheric aerosol budget from 22 years
of ground-based lidar and satellite observations, Atmos. Chem. Phys., 17,
1829–1845, <ext-link xlink:href="https://doi.org/10.5194/acp-17-1829-2017" ext-link-type="DOI">10.5194/acp-17-1829-2017</ext-link>, 2017.</mixed-citation></ref>
      <ref id="bib1.bib17"><label>17</label><mixed-citation>Kuttippurath, J., Lefèvre, F., Pommereau, J.-P., Roscoe, H. K., Goutail,
F., Pazmiño, A., and Shanklin, J. D.: Antarctic ozone loss in 1979–2010:
first sign of ozone recovery, Atmos. Chem. Phys., 13, 1625–1635,
<ext-link xlink:href="https://doi.org/10.5194/acp-13-1625-2013" ext-link-type="DOI">10.5194/acp-13-1625-2013</ext-link>, 2013.</mixed-citation></ref>
      <ref id="bib1.bib18"><label>18</label><mixed-citation>Kuttippurath, J., Godin-Beekmann, S., Lefèvre, F., Santee, M. L.,
Froidevaux, L., and Hauchecorne, A.: Variability in Antarctic ozone loss in
the last decade (2004–2013): high-resolution simulations compared to Aura
MLS observations, Atmos. Chem. Phys., 15, 10385–10397,
<ext-link xlink:href="https://doi.org/10.5194/acp-15-10385-2015" ext-link-type="DOI">10.5194/acp-15-10385-2015</ext-link>, 2015.</mixed-citation></ref>
      <ref id="bib1.bib19"><label>19</label><mixed-citation>
Levelt, P. F., van den Oord, G. H. J., Dobber, M. R., Mälkki, A., Visser,
H., de Vries, J., Stammes, P., Lundell, J. O. V., and Saari, H.: The Ozone
Monitoring Instrument, IEEE T. Geosci. Remote, 44, 1093–1101, 2006.</mixed-citation></ref>
      <ref id="bib1.bib20"><label>20</label><mixed-citation>McIntyre, M. and Palmer, T.: The “surf zone” in the stratosphere, J. Atmos.
Terr. Phys., 46, 825–849, <ext-link xlink:href="https://doi.org/10.1016/0021-9169(84)90063-1" ext-link-type="DOI">10.1016/0021-9169(84)90063-1</ext-link>, 1984.</mixed-citation></ref>
      <ref id="bib1.bib21"><label>21</label><mixed-citation>McPeters, R., Kroon, M., Labow, G., Brinksma, E., Balis, D.,
Petropavlovskikh, I., Veefkind, J. P., Bhartia, P. K., and Levelt, P. F.:
Validation of the Aura Ozone Monitoring Instrument total column ozone
product, J. Geophys. Res., 113, D15S14, <ext-link xlink:href="https://doi.org/10.1029/2007JD008802" ext-link-type="DOI">10.1029/2007JD008802</ext-link>, 2008.</mixed-citation></ref>
      <ref id="bib1.bib22"><label>22</label><mixed-citation>
McPeters, R. D., Krueger, A. J., Bhartia, P. K., Herman, J. R., Wellemeyer,
C. G., Seftor, C. J., Jaross, G., Torres, O., Moy, L., Labow, G., Byerly, W.,
Taylor, S. L., Swissler, T., and Cebula, R. P.: Earth Probe Total Ozone
Mapping Spectrometer (TOMS) Data Products User's Guide, NASA Reference
Publication 1998-206895, NASA, Washington DC, 1998.</mixed-citation></ref>
      <ref id="bib1.bib23"><label>23</label><mixed-citation>Nair, P. J., Godin-Beekmann, S., Kuttippurath, J., Ancellet, G., Goutail, F.,
Pazmiño, A., Froidevaux, L., Zawodny, J. M., Evans, R. D., Wang, H. J.,
Anderson, J., and Pastel, M.: Ozone trends derived from the total column and
vertical profiles at a northern mid-latitude station, Atmos. Chem. Phys., 13,
10373–10384, <ext-link xlink:href="https://doi.org/10.5194/acp-13-10373-2013" ext-link-type="DOI">10.5194/acp-13-10373-2013</ext-link>, 2013.</mixed-citation></ref>
      <ref id="bib1.bib24"><label>24</label><mixed-citation>Nash, E. R., Newman, P. A., Rosenfield, J. E., and Schoeberl, M. R.: An
objective determination of the polar vortex using Ertel's potential
vorticity, J. Geophys. Res., 101, 9471–9478, <ext-link xlink:href="https://doi.org/10.1029/96JD00066" ext-link-type="DOI">10.1029/96JD00066</ext-link>, 1996.</mixed-citation></ref>
      <ref id="bib1.bib25"><label>25</label><mixed-citation>Newman, P. A., Nash, E. R., Kawa, S. R., Montzka, S. A., and Schauffler, S.
M.: When will the Antarctic ozone hole recover?, Geophys. Res. Lett., 33,
L12814, <ext-link xlink:href="https://doi.org/10.1029/2005GL025232" ext-link-type="DOI">10.1029/2005GL025232</ext-link>, 2006.</mixed-citation></ref>
      <ref id="bib1.bib26"><label>26</label><mixed-citation>Newman, P. A., Daniel, J. S., Waugh, D. W., and Nash, E. R.: A new
formulation of equivalent effective stratospheric chlorine (EESC), Atmos.
Chem. Phys., 7, 4537–4552, <ext-link xlink:href="https://doi.org/10.5194/acp-7-4537-2007" ext-link-type="DOI">10.5194/acp-7-4537-2007</ext-link>, 2007.</mixed-citation></ref>
      <ref id="bib1.bib27"><label>27</label><mixed-citation>Pazmiño, A. F., Godin-Beekmann, S., Ginzburg, M., Bekki, S., Hauchecorne, A.,
Piacentini, R., and Quel, E.: Impact of Antarctic polar vortex occurrences on
total ozone and UVB radiation at southern Argentinean and Antarctic stations
during 1997–2003 period, J. Geophys. Res., 110, D03103,
<ext-link xlink:href="https://doi.org/10.1029/2004JD005304" ext-link-type="DOI">10.1029/2004JD005304</ext-link>, 2005.</mixed-citation></ref>
      <ref id="bib1.bib28"><label>28</label><mixed-citation>Pazmiño, A. F., Godin-Beekmann, S., Luccini, E. A., Piacentini, R. D.,
Quel, E. J., and Hauchecorne, A.: Increased UV radiation<?pagebreak page7572?> due to polar ozone
chemical depletion and vortex occurrences at Southern Sub-polar Latitudes in
the period [1997–2005], Atmos. Chem. Phys., 8, 5339–5352,
<ext-link xlink:href="https://doi.org/10.5194/acp-8-5339-2008" ext-link-type="DOI">10.5194/acp-8-5339-2008</ext-link>, 2008.</mixed-citation></ref>
      <ref id="bib1.bib29"><label>29</label><mixed-citation>Reinsel, G. C., Weatherhead, E. C., Tiao, G. C., Miller, A. J., Nagatani, R.
M., Wuebbles, D. J., and Flynn, L. E.: On detection of turnaround and
recovery in trend for ozone, J. Geophys. Res., 107, 4078,
<ext-link xlink:href="https://doi.org/10.1029/2001JD000500" ext-link-type="DOI">10.1029/2001JD000500</ext-link>, 2002.</mixed-citation></ref>
      <ref id="bib1.bib30"><label>30</label><mixed-citation>Salby, M. L., Titova, E. A., and Deschamps, L.: Changes of the Antarctic
ozone hole: Controlling mechanisms, seasonal predictability, and evolution,
J. Geophys. Res., 117, D10111, <ext-link xlink:href="https://doi.org/10.1029/2011JD016285" ext-link-type="DOI">10.1029/2011JD016285</ext-link>, 2012.</mixed-citation></ref>
      <ref id="bib1.bib31"><label>31</label><mixed-citation>Sato, M., Hansen, J. E., McCormick, M. P., and Pollack, J. B.: Stratospheric
aerosol optical depth, 1850–1990, J. Geophys. Res., 98, 22987–22994,
<ext-link xlink:href="https://doi.org/10.1029/93JD02553" ext-link-type="DOI">10.1029/93JD02553</ext-link>, 1993.</mixed-citation></ref>
      <ref id="bib1.bib32"><label>32</label><mixed-citation>Solomon, S., Ivy, D. J., Kinnison, D., Mills, M. J., Neely, R. R., and
Schmidt, A.: Emergence of healing in the Antarctic ozone layer,
Science,  353,  269–274,
<ext-link xlink:href="https://doi.org/10.1126/science.aae0061" ext-link-type="DOI">10.1126/science.aae0061</ext-link>, 2016.</mixed-citation></ref>
      <ref id="bib1.bib33"><label>33</label><mixed-citation>Solomon, S., Ivy, D., Gupta, M., Bandoro, J., Santer, B., Fu, Q., Lin, P.,
Garcia, R. R., Kinnison, D., and Mills, M.: Mirrored changes in Antarctic
ozone and stratospheric temperature in the late 20th versus early 21st
centuries, J. Geophys. Res.-Atmos., 122, 8940–8950,
<ext-link xlink:href="https://doi.org/10.1002/2017JD026719" ext-link-type="DOI">10.1002/2017JD026719</ext-link>, 2017.</mixed-citation></ref>
      <ref id="bib1.bib34"><label>34</label><mixed-citation>Steinbrecht, W., Hassler, B., Claude, H., Winkler, P., and Stolarski, R. S.:
Global distribution of total ozone and lower stratospheric temperature
variations, Atmos. Chem. Phys., 3, 1421–1438,
<ext-link xlink:href="https://doi.org/10.5194/acp-3-1421-2003" ext-link-type="DOI">10.5194/acp-3-1421-2003</ext-link>, 2003.
</mixed-citation></ref><?xmltex \hack{\newpage}?>
      <ref id="bib1.bib35"><label>35</label><mixed-citation>van der A, R. J., Allaart, M. A. F., and Eskes, H. J.: Multi sensor
reanalysis of total ozone, Atmos. Chem. Phys., 10, 11277–11294,
<ext-link xlink:href="https://doi.org/10.5194/acp-10-11277-2010" ext-link-type="DOI">10.5194/acp-10-11277-2010</ext-link>, 2010.</mixed-citation></ref>
      <ref id="bib1.bib36"><label>36</label><mixed-citation>van der A, R. J., Allaart, M. A. F., and Eskes, H. J.: Extended and refined
multi sensor reanalysis of total ozone for the period 1970–2012, Atmos. Meas.
Tech., 8, 3021–3035, <ext-link xlink:href="https://doi.org/10.5194/amt-8-3021-2015" ext-link-type="DOI">10.5194/amt-8-3021-2015</ext-link>, 2015.</mixed-citation></ref>
      <ref id="bib1.bib37"><label>37</label><mixed-citation>Weber, M., Coldewey-Egbers, M., Fioletov, V. E., Frith, S. M., Wild, J. D.,
Burrows, J. P., Long, C. S., and Loyola, D.: Total ozone trends from 1979 to
2016 derived from five merged observational datasets – the emergence into
ozone recovery, Atmos. Chem. Phys., 18, 2097–2117,
<ext-link xlink:href="https://doi.org/10.5194/acp-18-2097-2018" ext-link-type="DOI">10.5194/acp-18-2097-2018</ext-link>, 2018.</mixed-citation></ref>
      <ref id="bib1.bib38"><label>38</label><mixed-citation>
WMO (World Meteorological Organization): Scientific assessment of ozone
depletion: 2006, Global Ozone Research and Monitoring Project-Report 50,
Geneva, Switzerland, 2007.</mixed-citation></ref>
      <ref id="bib1.bib39"><label>39</label><mixed-citation>
WMO (World Meteorological Organisation): Scientific assessment of ozone
depletion: 2010, Global Ozone Research and Monitoring Project, Report 52,
Geneva, Switzerland, 516 pp., 2011.</mixed-citation></ref>
      <ref id="bib1.bib40"><label>40</label><mixed-citation>
WMO (World Meteorological Organization): Scientific Assessment of Ozone
Depletion: 2014, Global Ozone Research and Monitoring Project, Report No. 55,
Geneva, Switzerland, 416 pp., 2014.</mixed-citation></ref>
      <ref id="bib1.bib41"><label>41</label><mixed-citation>Yang, E.-S., Cunnold, D. M., Newchurch, M. J., Salawitch, R. J., McCormick,
M. P., Russell, J. M., Zawodny, J. M., and Oltmans, S. J.: First stage of
Antarctic ozone recovery, J. Geophys. Res., 113, D20308,
<ext-link xlink:href="https://doi.org/10.1029/2007JD009675" ext-link-type="DOI">10.1029/2007JD009675</ext-link>, 2008.</mixed-citation></ref>

  </ref-list></back>
    <!--<article-title-html>Multiple symptoms of total ozone recovery inside the Antarctic vortex during austral spring</article-title-html>
<abstract-html><p>The long-term evolution of total ozone column inside the Antarctic polar
vortex is investigated over the 1980–2017 period. Trend analyses are
performed using a multilinear regression (MLR) model based on various proxies
for the evaluation of ozone interannual variability (heat flux,
quasi-biennial oscillation, solar flux, Antarctic oscillation and aerosols).
Annual total ozone column measurements corresponding to the mean monthly values inside the
vortex in September and during the period of maximum ozone depletion from
15 September   to 15 October   are used. Total ozone columns from
the Multi-Sensor Reanalysis version 2 (MSR-2) dataset and from a combined record based
on TOMS and OMI satellite datasets with gaps filled by MSR-2 (1993–1995)
are considered in the study. Ozone trends are computed by a piece-wise
trend (PWT) proxy  that includes two linear functions before and after the
turnaround year in 2001 and a parabolic function to account for the
saturation of the polar ozone destruction. In order to evaluate average total
ozone within the vortex, two classification methods are used, based on the
potential vorticity gradient as a function of equivalent latitude. The first
standard one considers this gradient at a single isentropic level (475  or
550&thinsp;K), while the second one uses a range of isentropic levels between 400
and 600&thinsp;K. The regression model includes a new proxy (GRAD) linked to the
gradient of potential vorticity as a function of equivalent latitude and
representing the stability of the vortex during the studied month. The
determination coefficient (<i>R</i><sup>2</sup>) between observations and modelled values
increases by  ∼ &thinsp;0.05 when this proxy is included in the MLR
model. Highest <i>R</i><sup>2</sup> (0.92–0.95) and minimum residuals are obtained for the
second classification method for both datasets and months.</p><p>Trends in September over the 2001–2017 period are statistically
significant at 2<i>σ</i> level with values ranging between 1.84&thinsp;±&thinsp;1.03
and 2.83&thinsp;±&thinsp;1.48&thinsp;DU&thinsp;yr<sup>−1</sup> depending on the methods and considered
proxies. This result confirms the recent studies of Antarctic ozone healing
during that month. Trends from 2001 are 2 to 3 times smaller than before the
turnaround year, as expected from the response to the slowly ozone-depleting
substances decrease in polar regions.</p><p>For the first time, significant trends are found for the period of maximum
ozone depletion. Estimated trends from 2001 for the 15 September–15 October period over
2001–2017 vary from 1.21&thinsp;±&thinsp;0.83 to 1.96&thinsp;DU&thinsp;±&thinsp;0.99&thinsp;yr<sup>−1</sup> and
are significant at 2<i>σ</i> level.</p><p>MLR analysis is also applied to the ozone mass deficit (OMD) metric for both
periods, considering a threshold at 220&thinsp;DU and total ozone columns south of
60°&thinsp;S. Significant trend values are observed for all cases and
periods. A decrease of OMD of 0.86&thinsp;±&thinsp;0.36  and 0.65&thinsp;±&thinsp;0.33&thinsp;Mt&thinsp;yr<sup>−1</sup>
since 2001 is observed in September and 15 September–15 October,
respectively.</p><p>Ozone recovery is also confirmed by a steady decrease of the relative area
of total ozone values lower than 175&thinsp;DU within the vortex in the
15 September–15 October period since 2010 and a delay in the occurrence of ozone levels
below 125&thinsp;DU since 2005.</p></abstract-html>
<ref-html id="bib1.bib1"><label>1</label><mixed-citation>
Allen, D., Bevilacqua, R., Nedoluha, G., Randall, C., and Manney, G.:
Unusual stratospheric transport and mixing during 2002 Antarctic winter,
Geophys. Res. Lett., 30, 1599, <a href="https://doi.org/10.1029/2003GL017117" target="_blank">https://doi.org/10.1029/2003GL017117</a>, 2003.
</mixed-citation></ref-html>
<ref-html id="bib1.bib2"><label>2</label><mixed-citation>
Bhartia, P. K. and Wellemeyer, C.: TOMS-V8 total O3 algorithm, in OMI
Algorithm Theoretical Basis Document, vol. II, OMI Ozone Products, edited
by: P. K. Bhartia,  15–31, NASA Goddard Space Flight Center, Greenbelt,
Maryland, USA, 2002.
</mixed-citation></ref-html>
<ref-html id="bib1.bib3"><label>3</label><mixed-citation>
Bodeker, G. E. and Scourfield, M. W. J.: Planetary waves in total ozone and
their relation to Antarctic ozone depletion, Geophys. Res. Lett., 22,
2949–2952, 1995.
</mixed-citation></ref-html>
<ref-html id="bib1.bib4"><label>4</label><mixed-citation>
Bodeker, G. E., Struthers, H., and Connor, B. J.: Dynamical containment of
Antarctic ozone depletion, Geophys. Res. Lett., 29, 1098,
<a href="https://doi.org/10.1029/2001GL014206" target="_blank">https://doi.org/10.1029/2001GL014206</a>, 2002.
</mixed-citation></ref-html>
<ref-html id="bib1.bib5"><label>5</label><mixed-citation>
Chipperfield, M., Bekki, S., Dhomse, S., Harris, N. R. P., Hassler, B.,
Hossaini, R., Steinbrecht, W., Thiéblemont, R., and Weber, M.: Detecting
recovery of stratospheric ozone layer, Nature, 549, 211–218,
<a href="https://doi.org/10.1038/nature23681" target="_blank">https://doi.org/10.1038/nature23681</a>, 2017.
</mixed-citation></ref-html>
<ref-html id="bib1.bib6"><label>6</label><mixed-citation>
Chubachi, S.: A special observation at Syowa station, Antarctica from
February 1982 to January 1983, in: Atmospheric Ozone, edited by: Zerefos, C.
and A. Ghazi, Springer, the Netherlands, 285–289,
<a href="https://doi.org/10.1007/978-94-009-5313-0_58" target="_blank">https://doi.org/10.1007/978-94-009-5313-0_58</a>, 1985.
</mixed-citation></ref-html>
<ref-html id="bib1.bib7"><label>7</label><mixed-citation>
Farman, J. C., Gardiner, B. G., and Shanklin, J. D.: Large losses of total
ozone in Antarctica reveal seasonal ClOx/NOx interaction, Nature, 315,
207–210, <a href="https://doi.org/10.1038/315207a0" target="_blank">https://doi.org/10.1038/315207a0</a>, 1985.
</mixed-citation></ref-html>
<ref-html id="bib1.bib8"><label>8</label><mixed-citation>
Dee, D. P., Uppala, S. M., Simmons, A. J., Berrisford, P., Poli, P.,
Kobayashi, S., Andrae, U., Balmaseda, M. A., Balsamo, G., Bauer, P.,
Bechtold, P., Beljaars, A. C. M., van de Berg, L., Bidlot, J., Bormann, N.,
Delsol, C., Dragani, R., Fuentes, M., Geer, A. J., Haimberger, L., Healy, S.
B., Hersbach, H., Hólm, E. V., Isaksen, L., Kållberg, P., Köhler,
M., Matricardi, M., McNally, A. P., Monge-Sanz, B. M., Morcrette, J.-J.,
Park, B.-K., Peubey, C., de Rosnay, P., Tavolato, C., Thépaut, J.-N., and
Vitart, F.: The ERA-Interim reanalysis: configuration and performance of the
data assimilation system, Q. J. R. Meteorol. Soc., 137, 553–597,
<a href="https://doi.org/10.1002/qj.828" target="_blank">https://doi.org/10.1002/qj.828</a>, 2011.
</mixed-citation></ref-html>
<ref-html id="bib1.bib9"><label>9</label><mixed-citation>
de Laat, A. T. J. and van Weele, M.: The 2010 Antarctic ozone hole: Observed
reduction in ozone destruction by minor sudden stratospheric warmings, Sci.
Rep., 1, 38,
<a href="https://doi.org/10.1038/srep00038" target="_blank">https://doi.org/10.1038/srep00038</a>, 2011.
</mixed-citation></ref-html>
<ref-html id="bib1.bib10"><label>10</label><mixed-citation>
de Laat, A. T. J., van der A, R. J., and van Weele, M.: Tracing the second
stage of ozone recovery in the Antarctic ozone-hole with a “big data”
approach to multivariate regressions, Atmos. Chem. Phys., 15, 79–97,
<a href="https://doi.org/10.5194/acp-15-79-2015" target="_blank">https://doi.org/10.5194/acp-15-79-2015</a>, 2015.
</mixed-citation></ref-html>
<ref-html id="bib1.bib11"><label>11</label><mixed-citation>
de Laat, A. T. J., van Weele, M., and van der A, R. J.: Onset of
Stratospheric Ozone Recovery in the Antarctic Ozone Hole in Assimilated
Daily Total Ozone Columns, J. Geophys. Res., 122, 11880–11899,
<a href="https://doi.org/10.1002/2016JD025723" target="_blank">https://doi.org/10.1002/2016JD025723</a>,   2017.
</mixed-citation></ref-html>
<ref-html id="bib1.bib12"><label>12</label><mixed-citation>
Godin, S., Bergeret, V., Bekki, S., David, C., and Mégie, G.: Study of
the interannual ozone loss and the permeability of the Antarctic polar vortex
from aerosols and ozone lidar measurements in Dumont d'Urville
(66.4°&thinsp;S, 140°&thinsp;E), J. Geophys. Res., 106, 1311–1330,
<a href="https://doi.org/10.1029/2000JD900459" target="_blank">https://doi.org/10.1029/2000JD900459</a>, 2001.
</mixed-citation></ref-html>
<ref-html id="bib1.bib13"><label>13</label><mixed-citation>
Hauchecorne, A., Chanin, M.-L., and Keckhut, P.: Climatology and trends of
the middle atmospheric temperature (33–87&thinsp;km) as seen by Rayleigh lidar
over the south of France, J. Geophys. Res., 96, 15297–15309,
<a href="https://doi.org/10.1029/91JD01213" target="_blank">https://doi.org/10.1029/91JD01213</a>, 1991.
</mixed-citation></ref-html>
<ref-html id="bib1.bib14"><label>14</label><mixed-citation>
Hauchecorne, A., Godin, S., Marchand, M., Heese, B., and Souprayen, C.:
Estimation of the Transport of Chemical Constituents from the Polar Vortex to
Middle Latitudes in the Lower Stratosphere using the High-Resolution
Advection Model MIMOSA and Effective Diffusivity, J. Geophys. Res., 107,
8289, <a href="https://doi.org/10.1029/2001JD000491" target="_blank">https://doi.org/10.1029/2001JD000491</a>, 2002.
</mixed-citation></ref-html>
<ref-html id="bib1.bib15"><label>15</label><mixed-citation>
Kerzenmacher, T. E., Keckhut, P., Hauchecorne, A., and Chanin, M.-L.:
Methodological uncertainties in multi-regression analyses of
middle-atmospheric data series, J. Environ. Monitor., 7, 682–690,
<a href="https://doi.org/10.1039/B603750J" target="_blank">https://doi.org/10.1039/B603750J</a>, 2006.
</mixed-citation></ref-html>
<ref-html id="bib1.bib16"><label>16</label><mixed-citation>
Khaykin, S. M., Godin-Beekmann, S., Keckhut, P., Hauchecorne, A., Jumelet,
J., Vernier, J.-P., Bourassa, A., Degenstein, D. A., Rieger, L. A., Bingen,
C., Vanhellemont, F., Robert, C., DeLand, M., and Bhartia, P. K.: Variability
and evolution of the midlatitude stratospheric aerosol budget from 22 years
of ground-based lidar and satellite observations, Atmos. Chem. Phys., 17,
1829–1845, <a href="https://doi.org/10.5194/acp-17-1829-2017" target="_blank">https://doi.org/10.5194/acp-17-1829-2017</a>, 2017.
</mixed-citation></ref-html>
<ref-html id="bib1.bib17"><label>17</label><mixed-citation>
Kuttippurath, J., Lefèvre, F., Pommereau, J.-P., Roscoe, H. K., Goutail,
F., Pazmiño, A., and Shanklin, J. D.: Antarctic ozone loss in 1979–2010:
first sign of ozone recovery, Atmos. Chem. Phys., 13, 1625–1635,
<a href="https://doi.org/10.5194/acp-13-1625-2013" target="_blank">https://doi.org/10.5194/acp-13-1625-2013</a>, 2013.
</mixed-citation></ref-html>
<ref-html id="bib1.bib18"><label>18</label><mixed-citation>
Kuttippurath, J., Godin-Beekmann, S., Lefèvre, F., Santee, M. L.,
Froidevaux, L., and Hauchecorne, A.: Variability in Antarctic ozone loss in
the last decade (2004–2013): high-resolution simulations compared to Aura
MLS observations, Atmos. Chem. Phys., 15, 10385–10397,
<a href="https://doi.org/10.5194/acp-15-10385-2015" target="_blank">https://doi.org/10.5194/acp-15-10385-2015</a>, 2015.
</mixed-citation></ref-html>
<ref-html id="bib1.bib19"><label>19</label><mixed-citation>
Levelt, P. F., van den Oord, G. H. J., Dobber, M. R., Mälkki, A., Visser,
H., de Vries, J., Stammes, P., Lundell, J. O. V., and Saari, H.: The Ozone
Monitoring Instrument, IEEE T. Geosci. Remote, 44, 1093–1101, 2006.
</mixed-citation></ref-html>
<ref-html id="bib1.bib20"><label>20</label><mixed-citation>
McIntyre, M. and Palmer, T.: The “surf zone” in the stratosphere, J. Atmos.
Terr. Phys., 46, 825–849, <a href="https://doi.org/10.1016/0021-9169(84)90063-1" target="_blank">https://doi.org/10.1016/0021-9169(84)90063-1</a>, 1984.
</mixed-citation></ref-html>
<ref-html id="bib1.bib21"><label>21</label><mixed-citation>
McPeters, R., Kroon, M., Labow, G., Brinksma, E., Balis, D.,
Petropavlovskikh, I., Veefkind, J. P., Bhartia, P. K., and Levelt, P. F.:
Validation of the Aura Ozone Monitoring Instrument total column ozone
product, J. Geophys. Res., 113, D15S14, <a href="https://doi.org/10.1029/2007JD008802" target="_blank">https://doi.org/10.1029/2007JD008802</a>, 2008.
</mixed-citation></ref-html>
<ref-html id="bib1.bib22"><label>22</label><mixed-citation>
McPeters, R. D., Krueger, A. J., Bhartia, P. K., Herman, J. R., Wellemeyer,
C. G., Seftor, C. J., Jaross, G., Torres, O., Moy, L., Labow, G., Byerly, W.,
Taylor, S. L., Swissler, T., and Cebula, R. P.: Earth Probe Total Ozone
Mapping Spectrometer (TOMS) Data Products User's Guide, NASA Reference
Publication 1998-206895, NASA, Washington DC, 1998.
</mixed-citation></ref-html>
<ref-html id="bib1.bib23"><label>23</label><mixed-citation>
Nair, P. J., Godin-Beekmann, S., Kuttippurath, J., Ancellet, G., Goutail, F.,
Pazmiño, A., Froidevaux, L., Zawodny, J. M., Evans, R. D., Wang, H. J.,
Anderson, J., and Pastel, M.: Ozone trends derived from the total column and
vertical profiles at a northern mid-latitude station, Atmos. Chem. Phys., 13,
10373–10384, <a href="https://doi.org/10.5194/acp-13-10373-2013" target="_blank">https://doi.org/10.5194/acp-13-10373-2013</a>, 2013.
</mixed-citation></ref-html>
<ref-html id="bib1.bib24"><label>24</label><mixed-citation>
Nash, E. R., Newman, P. A., Rosenfield, J. E., and Schoeberl, M. R.: An
objective determination of the polar vortex using Ertel's potential
vorticity, J. Geophys. Res., 101, 9471–9478, <a href="https://doi.org/10.1029/96JD00066" target="_blank">https://doi.org/10.1029/96JD00066</a>, 1996.
</mixed-citation></ref-html>
<ref-html id="bib1.bib25"><label>25</label><mixed-citation>
Newman, P. A., Nash, E. R., Kawa, S. R., Montzka, S. A., and Schauffler, S.
M.: When will the Antarctic ozone hole recover?, Geophys. Res. Lett., 33,
L12814, <a href="https://doi.org/10.1029/2005GL025232" target="_blank">https://doi.org/10.1029/2005GL025232</a>, 2006.
</mixed-citation></ref-html>
<ref-html id="bib1.bib26"><label>26</label><mixed-citation>
Newman, P. A., Daniel, J. S., Waugh, D. W., and Nash, E. R.: A new
formulation of equivalent effective stratospheric chlorine (EESC), Atmos.
Chem. Phys., 7, 4537–4552, <a href="https://doi.org/10.5194/acp-7-4537-2007" target="_blank">https://doi.org/10.5194/acp-7-4537-2007</a>, 2007.
</mixed-citation></ref-html>
<ref-html id="bib1.bib27"><label>27</label><mixed-citation>
Pazmiño, A. F., Godin-Beekmann, S., Ginzburg, M., Bekki, S., Hauchecorne, A.,
Piacentini, R., and Quel, E.: Impact of Antarctic polar vortex occurrences on
total ozone and UVB radiation at southern Argentinean and Antarctic stations
during 1997–2003 period, J. Geophys. Res., 110, D03103,
<a href="https://doi.org/10.1029/2004JD005304" target="_blank">https://doi.org/10.1029/2004JD005304</a>, 2005.
</mixed-citation></ref-html>
<ref-html id="bib1.bib28"><label>28</label><mixed-citation>
Pazmiño, A. F., Godin-Beekmann, S., Luccini, E. A., Piacentini, R. D.,
Quel, E. J., and Hauchecorne, A.: Increased UV radiation due to polar ozone
chemical depletion and vortex occurrences at Southern Sub-polar Latitudes in
the period [1997–2005], Atmos. Chem. Phys., 8, 5339–5352,
<a href="https://doi.org/10.5194/acp-8-5339-2008" target="_blank">https://doi.org/10.5194/acp-8-5339-2008</a>, 2008.
</mixed-citation></ref-html>
<ref-html id="bib1.bib29"><label>29</label><mixed-citation>
Reinsel, G. C., Weatherhead, E. C., Tiao, G. C., Miller, A. J., Nagatani, R.
M., Wuebbles, D. J., and Flynn, L. E.: On detection of turnaround and
recovery in trend for ozone, J. Geophys. Res., 107, 4078,
<a href="https://doi.org/10.1029/2001JD000500" target="_blank">https://doi.org/10.1029/2001JD000500</a>, 2002.
</mixed-citation></ref-html>
<ref-html id="bib1.bib30"><label>30</label><mixed-citation>
Salby, M. L., Titova, E. A., and Deschamps, L.: Changes of the Antarctic
ozone hole: Controlling mechanisms, seasonal predictability, and evolution,
J. Geophys. Res., 117, D10111, <a href="https://doi.org/10.1029/2011JD016285" target="_blank">https://doi.org/10.1029/2011JD016285</a>, 2012.
</mixed-citation></ref-html>
<ref-html id="bib1.bib31"><label>31</label><mixed-citation>
Sato, M., Hansen, J. E., McCormick, M. P., and Pollack, J. B.: Stratospheric
aerosol optical depth, 1850–1990, J. Geophys. Res., 98, 22987–22994,
<a href="https://doi.org/10.1029/93JD02553" target="_blank">https://doi.org/10.1029/93JD02553</a>, 1993.
</mixed-citation></ref-html>
<ref-html id="bib1.bib32"><label>32</label><mixed-citation>
Solomon, S., Ivy, D. J., Kinnison, D., Mills, M. J., Neely, R. R., and
Schmidt, A.: Emergence of healing in the Antarctic ozone layer,
Science,  353,  269–274,
<a href="https://doi.org/10.1126/science.aae0061" target="_blank">https://doi.org/10.1126/science.aae0061</a>, 2016.
</mixed-citation></ref-html>
<ref-html id="bib1.bib33"><label>33</label><mixed-citation>
Solomon, S., Ivy, D., Gupta, M., Bandoro, J., Santer, B., Fu, Q., Lin, P.,
Garcia, R. R., Kinnison, D., and Mills, M.: Mirrored changes in Antarctic
ozone and stratospheric temperature in the late 20th versus early 21st
centuries, J. Geophys. Res.-Atmos., 122, 8940–8950,
<a href="https://doi.org/10.1002/2017JD026719" target="_blank">https://doi.org/10.1002/2017JD026719</a>, 2017.
</mixed-citation></ref-html>
<ref-html id="bib1.bib34"><label>34</label><mixed-citation>
Steinbrecht, W., Hassler, B., Claude, H., Winkler, P., and Stolarski, R. S.:
Global distribution of total ozone and lower stratospheric temperature
variations, Atmos. Chem. Phys., 3, 1421–1438,
<a href="https://doi.org/10.5194/acp-3-1421-2003" target="_blank">https://doi.org/10.5194/acp-3-1421-2003</a>, 2003.

</mixed-citation></ref-html>
<ref-html id="bib1.bib35"><label>35</label><mixed-citation>
van der A, R. J., Allaart, M. A. F., and Eskes, H. J.: Multi sensor
reanalysis of total ozone, Atmos. Chem. Phys., 10, 11277–11294,
<a href="https://doi.org/10.5194/acp-10-11277-2010" target="_blank">https://doi.org/10.5194/acp-10-11277-2010</a>, 2010.
</mixed-citation></ref-html>
<ref-html id="bib1.bib36"><label>36</label><mixed-citation>
van der A, R. J., Allaart, M. A. F., and Eskes, H. J.: Extended and refined
multi sensor reanalysis of total ozone for the period 1970–2012, Atmos. Meas.
Tech., 8, 3021–3035, <a href="https://doi.org/10.5194/amt-8-3021-2015" target="_blank">https://doi.org/10.5194/amt-8-3021-2015</a>, 2015.
</mixed-citation></ref-html>
<ref-html id="bib1.bib37"><label>37</label><mixed-citation>
Weber, M., Coldewey-Egbers, M., Fioletov, V. E., Frith, S. M., Wild, J. D.,
Burrows, J. P., Long, C. S., and Loyola, D.: Total ozone trends from 1979 to
2016 derived from five merged observational datasets – the emergence into
ozone recovery, Atmos. Chem. Phys., 18, 2097–2117,
<a href="https://doi.org/10.5194/acp-18-2097-2018" target="_blank">https://doi.org/10.5194/acp-18-2097-2018</a>, 2018.
</mixed-citation></ref-html>
<ref-html id="bib1.bib38"><label>38</label><mixed-citation>
WMO (World Meteorological Organization): Scientific assessment of ozone
depletion: 2006, Global Ozone Research and Monitoring Project-Report 50,
Geneva, Switzerland, 2007.
</mixed-citation></ref-html>
<ref-html id="bib1.bib39"><label>39</label><mixed-citation>
WMO (World Meteorological Organisation): Scientific assessment of ozone
depletion: 2010, Global Ozone Research and Monitoring Project, Report 52,
Geneva, Switzerland, 516 pp., 2011.
</mixed-citation></ref-html>
<ref-html id="bib1.bib40"><label>40</label><mixed-citation>
WMO (World Meteorological Organization): Scientific Assessment of Ozone
Depletion: 2014, Global Ozone Research and Monitoring Project, Report No. 55,
Geneva, Switzerland, 416 pp., 2014.
</mixed-citation></ref-html>
<ref-html id="bib1.bib41"><label>41</label><mixed-citation>
Yang, E.-S., Cunnold, D. M., Newchurch, M. J., Salawitch, R. J., McCormick,
M. P., Russell, J. M., Zawodny, J. M., and Oltmans, S. J.: First stage of
Antarctic ozone recovery, J. Geophys. Res., 113, D20308,
<a href="https://doi.org/10.1029/2007JD009675" target="_blank">https://doi.org/10.1029/2007JD009675</a>, 2008.
</mixed-citation></ref-html>--></article>
