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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-21-6811-2021</article-id><title-group><article-title>Analysis of recent lower-stratospheric ozone trends<?xmltex \hack{\break}?> in chemistry climate models</article-title><alt-title>Analysis of recent lower-stratospheric ozone trends in chemistry climate models</alt-title>
      </title-group><?xmltex \runningtitle{Analysis of recent lower-stratospheric ozone trends in chemistry climate models}?><?xmltex \runningauthor{S.~Dietm\"{u}ller et~al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Dietmüller</surname><given-names>Simone</given-names></name>
          <email>simone.dietmueller@dlr.de</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Garny</surname><given-names>Hella</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2 aff1 aff3">
          <name><surname>Eichinger</surname><given-names>Roland</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6872-5700</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4 aff5 aff6">
          <name><surname>Ball</surname><given-names>William T.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1005-3670</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Deutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, Oberpfaffenhofen, Germany</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Ludwig Maximilians Universität, Faculty of Physics, Institute for Meteorology, Munich, Germany</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Charles University, Department of Atmospheric Physics, Faculty of Mathematics and Physics, Prague, Czech Republic</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Institute for Atmospheric and Climate Science, Swiss Federal Institute of Technology Zurich, Zurich, Switzerland</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>Physikalisch-Meteorologisches Observatorium Davos World Radiation Centre,<?xmltex \hack{\break}?> Dorfstrasse 33, 7260 Davos Dorf, Switzerland</institution>
        </aff>
        <aff id="aff6"><label>6</label><institution>Department of Geoscience and Remote Sensing, Faculty of Civil Engineering and Geosciences,<?xmltex \hack{\break}?> TU Delft, Stevinweg 1, 2628 CN Delft, the Netherlands</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Simone Dietmüller
(simone.dietmueller@dlr.de)</corresp></author-notes><pub-date><day>5</day><month>May</month><year>2021</year></pub-date>
      
      <volume>21</volume>
      <issue>9</issue>
      <fpage>6811</fpage><lpage>6837</lpage>
      <history>
        <date date-type="received"><day>9</day><month>September</month><year>2020</year></date>
           <date date-type="accepted"><day>12</day><month>March</month><year>2021</year></date>
           <date date-type="rev-recd"><day>17</day><month>February</month><year>2021</year></date>
           <date date-type="rev-request"><day>12</day><month>October</month><year>2020</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2021 </copyright-statement>
        <copyright-year>2021</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><title>Abstract</title>
    <p id="d1e149">Recent observations show a significant decrease in lower-stratospheric (LS)
ozone concentrations in tropical and mid-latitude regions since 1998. By
analysing 31 chemistry climate model (CCM) simulations performed for the
Chemistry Climate Model Initiative (CCMI; <xref ref-type="bibr" rid="bib1.bibx55" id="altparen.1"/>), we find
a large spread in the 1998–2018 trend patterns between different CCMs and
between different realizations performed with the same CCM. The latter in
particular indicates that natural variability strongly influences LS ozone
trends. However none of the model simulations reproduce the observed ozone
trend structure of coherent negative trends in the LS. In contrast to the
observations, most models show an LS trend pattern with negative trends in the
tropics (20<inline-formula><mml:math id="M1" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–20<inline-formula><mml:math id="M2" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) and positive trends in the northern
mid-latitudes (30–50<inline-formula><mml:math id="M3" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) or vice versa. To investigate the influence
of natural variability on recent LS ozone trends, we analyse the
sensitivity of observational trends and the models' trend probability
distributions for varying periods with start dates from 1995 to 2001 and
end dates from 2013 to 2019. Generally, modelled and observed LS trends
remain robust for these different periods; however observational data show a
change towards weaker mid-latitude trends for certain periods, likely forced
by natural variability. Moreover we show that in the tropics the observed
trends agree well with the models' trend distribution, whereas in the
mid-latitudes the observational trend is typically an extreme value of the
models' distribution. We further investigate the LS ozone trends for extended
periods reaching into the future and find that all models develop a positive
ozone trend at mid-latitudes, and the trends converge to constant values by the
period that spans 1998–2060. Inter-model correlations between ozone trends and transport-circulation trends confirm the dominant role of
greenhouse gas (GHG)-driven tropical upwelling enhancement on the tropical LS
ozone decrease. Mid-latitude ozone, on the other hand, appears to be
influenced by multiple competing factors: an enhancement in the shallow branch
decreases ozone, while an enhancement in the deep branch increases ozone, and,
furthermore, mixing plays a role here too. Sensitivity simulations with fixed
forcing of GHGs or ozone-depleting substances (ODSs) reveal that the
GHG-driven increase in circulation strength does not lead to a net trend in LS
mid-latitude column ozone. Rather, the positive ozone trends simulated
consistently in the models in this region emerge from the decline in ODSs,
i.e. the ozone recovery. Therefore, we hypothesize that next to the influence
of natural variability, the disagreement of modelled and observed LS
mid-latitude ozone trends could indicate a mismatch in the relative role of
the response of ozone to ODS versus GHG forcing in the models.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<?pagebreak page6812?><sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e191">Stratospheric ozone is essential for protecting the Earth's surface from ultraviolet radiation, which is harmful for plants, animals, and humans. Human-made
ozone-depleting-substance (ODS) emissions significantly reduced ozone
concentrations for some decades after 1960. After controlling the use of ODSs
by the 1987 Montreal Protocol and later adjustments, however, ODS
concentrations started to decline in the mid to late 1990s
<xref ref-type="bibr" rid="bib1.bibx57 bib1.bibx17" id="paren.2"><named-content content-type="pre">e.g.</named-content></xref>. As a consequence, total
stratospheric ozone is expected to recover in the future. <xref ref-type="bibr" rid="bib1.bibx22" id="text.3"/>
have analysed the recovery of stratospheric ozone mixing ratios of the CCMI-1
(Chemistry Climate Model Intercomparison project part 1) climate projection
simulations. They found that the ozone layer is simulated to return to a
pre-1980 ODS level between 2030 and 2060, depending on the region. However,
they discovered a large spread among the individual models, which shows that
there are many uncertainties in these projections. The evolution of
stratospheric ozone in the 21st century results not only from a decrease
in ODS concentrations but also from an interplay between changes in both the
atmospheric composition and the circulation (World Meteorological Organization
(WMO) 2014). Increasing anthropogenic greenhouse gas (GHG) emissions
(<inline-formula><mml:math id="M4" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M5" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M6" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>) leads to enhanced tropical upwelling
and thereby to an acceleration of tracer transport along the stratospheric
overturning circulation <xref ref-type="bibr" rid="bib1.bibx13 bib1.bibx26" id="paren.4"><named-content content-type="pre">e.g.</named-content></xref>. On the
other hand, increasing GHG concentrations also slows down ozone depletion through
GHG-induced stratospheric cooling
<xref ref-type="bibr" rid="bib1.bibx41 bib1.bibx60 bib1.bibx10 bib1.bibx23 bib1.bibx48" id="paren.5"><named-content content-type="pre">e.g.</named-content></xref>, and
emissions of <inline-formula><mml:math id="M7" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M8" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula> additionally impact ozone through
chemical processes
<xref ref-type="bibr" rid="bib1.bibx71 bib1.bibx42 bib1.bibx74 bib1.bibx90" id="paren.6"><named-content content-type="pre">e.g.</named-content></xref>.</p>
      <p id="d1e277">In recent years, a number of studies have analysed observational records
to identify ozone trends in the stratosphere
<xref ref-type="bibr" rid="bib1.bibx33 bib1.bibx78 bib1.bibx89" id="paren.7"><named-content content-type="pre">e.g.</named-content></xref>. These studies
consistently report an ozone recovery in the upper stratosphere after the
turnaround of the ODS concentrations around the year 1998. In the lower
stratosphere (LS), however, most observed ozone trends are not statistically
significant for such a relatively short period due to large internal
variability and instrumental difficulties
<xref ref-type="bibr" rid="bib1.bibx78" id="paren.8"><named-content content-type="pre">e.g.</named-content></xref>. Subsequently, <xref ref-type="bibr" rid="bib1.bibx6" id="text.9"/> analysed LS
ozone trends from satellite data between 1998 and 2016 in detail, making use of
a dynamical (multiple) linear regression analysis. They identified a
statistically significant decline in LS ozone between 60<inline-formula><mml:math id="M9" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and
60<inline-formula><mml:math id="M10" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N in that period of approximately 2 <inline-formula><mml:math id="M11" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> in the LS below
24 <inline-formula><mml:math id="M12" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula> altitude. The implication was that the stratospheric ozone
column was continuing to decline because the LS ozone reduction more than
offsets the positive trend in the upper stratosphere. Shortly afterwards
<xref ref-type="bibr" rid="bib1.bibx87" id="text.10"/> studied ozone trends in the reanalysis products MERRA-2 and
GEOS-RPIT. In the tropics they detected a positive ozone trend in a
5 <inline-formula><mml:math id="M13" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula> layer above the tropopause and a negative trend at
7–15 <inline-formula><mml:math id="M14" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula> above the tropopause. Nevertheless, in the northern and
southern mid-latitude LS they detected a negative ozone trend. As such, there
are some similarities to the findings of <xref ref-type="bibr" rid="bib1.bibx6" id="text.11"/>, but there are also
quantitative differences, for example the positive trend in the 5 <inline-formula><mml:math id="M15" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula>
layer or a missing overall statistically significant decrease in the column
integrated ozone.  <xref ref-type="bibr" rid="bib1.bibx87" id="text.12"/> suggested that the negative mid-latitude
trend might be explained by enhanced isentropic transport between the tropical
and mid-latitude LS.  However, the recent study of <xref ref-type="bibr" rid="bib1.bibx63" id="text.13"/> explicitly
demonstrated that in the Northern Hemisphere (NH) this mid-latitude ozone decrease is primarily
associated with large-scale advection. Furthermore, they showed that the
observed changes in advection and in ozone are well within the range of model
variability (gauged from one chemistry climate model, CCM). By means of using a chemistry transport
model (CTM) and extending the analysis period to the year 2017,
<xref ref-type="bibr" rid="bib1.bibx18" id="text.14"/> suggested that the negative LS ozone trends are only
a result of large natural variability. They showed that there was a strong
positive ozone anomaly in 2017 which is driven by short-term dynamical
transport of ozone and concluded that this points to large year-to-year
variability rather than to an ongoing downward trend. However, an update of
the dataset which was used in <xref ref-type="bibr" rid="bib1.bibx6" id="text.15"/> showed that the large
interannual variability alone cannot explain the entire trend in
<xref ref-type="bibr" rid="bib1.bibx18" id="text.16"/> <xref ref-type="bibr" rid="bib1.bibx7" id="paren.17"><named-content content-type="pre">see</named-content></xref>: the larger year-to-year
variability in the Southern Hemisphere (SH) was implicated to result from a non-linear interaction
between the quasi-biennial oscillation (QBO) and seasonal variability, and
despite this large variability the observed negative LS ozone trend remains.</p>
      <p id="d1e380">To improve confidence in future projections of the ozone layer, it is important
to evaluate the skill of chemistry climate models (CCMs) in simulating the
observed ozone trends over recent decades. A direct comparison between the CCM
multi-model mean (MMM) values and observational data showed that the ozone
trend profiles of modelled MMM data agree well with observations, except in the
lowermost mid-latitude stratosphere <xref ref-type="bibr" rid="bib1.bibx77 bib1.bibx91" id="paren.18"/>. The most
recent study of <xref ref-type="bibr" rid="bib1.bibx8" id="text.19"/> investigated LS ozone trends of the
1998–2016 period in merged satellite data and compared them to the ozone
trends in CCMs using the climate projection simulations of the CCMVal2
project. Similar to the observations, the CCMs showed a decline in LS ozone in
the tropics, likely due to enhanced tropical upwelling, following from an
increase in greenhouse gases <xref ref-type="bibr" rid="bib1.bibx69" id="paren.20"><named-content content-type="pre">see e.g.</named-content></xref>. In contrast to
the observations, however, models do not show a decrease but rather an
increase in LS mid-latitude ozone. <xref ref-type="bibr" rid="bib1.bibx8" id="text.21"/> argue that these
discrepancies in the LS between models and observations can possibly be
explained by differences in the horizontal<?pagebreak page6813?> two-way mixing between the tropics
and mid-latitudes, though they did not provide explicit evidence from the
models <xref ref-type="bibr" rid="bib1.bibx87" id="paren.22"><named-content content-type="pre">see also</named-content></xref>. The study suggested that the negative
mid-latitude observational trend is caused by an intensification of two-way
mixing (by analysing effective diffusivity in reanalysis data). On the other
hand enhanced downwelling of ozone-rich air to the mid-latitudes could
consequently lead to a positive trend in the mid-latitudes. Apparently, the
processes that determine mid-latitude LS ozone in models and observations are
not fully understood.</p>
      <p id="d1e402">In the present study, we seek to quantify whether the observed LS ozone trends
lie within the suite of modelled trends. If yes, this would imply that the
observed trend is just one realization of possible trends given within the
large year-to-year variability. If not, this would imply either that models do
not represent year-to-year variability correctly or that there is a forced
trend in the real world that is not adequately represented in the models. In
contrast to the study of <xref ref-type="bibr" rid="bib1.bibx8" id="text.23"/>, we are using the simulation data of
a more recent inter-model comparison project (namely the Chemistry Climate
Model Initiative, phase 1, CCMI-1) and analyse the ozone trends for a wider
range of updated current state-of-the-art CCMs, including all their ensemble
simulations.</p>
      <p id="d1e409">A brief description of the model simulations, of the observational datasets,
and of the methods used is presented in Sect. <xref ref-type="sec" rid="Ch1.S2"/>. In
Sect. <xref ref-type="sec" rid="Ch1.S3"/> we show our results. We provide a detailed comparison
of ozone trends over the years 1998–2018 in different CCM simulations and
observations (Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>). Here we focus on LS ozone trends, and we
investigate how natural variability influences these LS ozone trends
(Sects. <xref ref-type="sec" rid="Ch1.S3.SS2"/> and <xref ref-type="sec" rid="Ch1.S3.SS3"/>). We link LS ozone trends
with stratospheric transport trends (Sect. <xref ref-type="sec" rid="Ch1.S3.SS4"/>), and we
investigate how ozone trends are forced by GHG and ODS emissions
(Sect. <xref ref-type="sec" rid="Ch1.S3.SS5"/>). A discussion of the reasons for the disagreement in
the LS mid-latitude ozone trends between models and observations and the
conclusions follow in Sects. <xref ref-type="sec" rid="Ch1.S4"/> and <xref ref-type="sec" rid="Ch1.S5"/>,
respectively.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Data and methods</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Models and simulations</title>
      <p id="d1e446">In the present study, we analyse the model output from 18 state-of-the-art
CCMs from the Chemistry Climate Model Initiative phase 1 (CCMI-1;
<xref ref-type="bibr" rid="bib1.bibx55" id="altparen.24"/>). Table <xref ref-type="table" rid="Ch1.T1"/> lists all these CCMs
together with their references, the forcing that underlies the sea surface
temperatures (SSTs), and the simulation type considered.  A detailed overview
of all models that participated in CCMI-1 can be found in
<xref ref-type="bibr" rid="bib1.bibx55" id="text.25"/>. We mainly evaluate the long-term “free-running”
simulations of CCMI-1 (REF-C2) as they span the time period 1998–2018. We do
not use REF-C1 free-running simulations of the recent past or the
specified dynamics simulations (REF-C1SD) as they only span the period from
1998 to 2010. Moreover we want to point out that the specified dynamics
simulations performed for CCMI do not represent stratospheric circulation
better than the free-running simulations: <xref ref-type="bibr" rid="bib1.bibx19" id="text.26"/> compared
stratospheric residual circulation among specified dynamic (SD) simulations
and found that the spread in these simulations is even larger than in
REF-C2. Furthermore <xref ref-type="bibr" rid="bib1.bibx6" id="text.27"/> showed poor agreement with the observed
ozone trend for some selected SD simulations of CCMI.  For the REF-C2 model
simulations used in our study, all available ensemble members of the
individual models are taken into account. The ensemble size of a certain
simulation (if ensemble simulations were performed) is also given in
Table <xref ref-type="table" rid="Ch1.T1"/> (brackets after simulations). Thus for the REF-C2
simulations, 18 models performed a total of 31 realizations (six models
performed multiple-ensemble-member simulations).  The REF-C2 simulations
include hindcast and forecast periods spanning 1960–2100. They are all free-running simulations; thus each model simulation has its own internal
variability. Note that REF-C2 simulations use a variety of different SSTs and
SICs (sea ice concentrations), either prescribed climate model SST fields from
offline model simulations (of the same or of a different model), or they are
coupled to an interactive ocean and sea ice module. Moreover the
representation of the QBO is different across the CCMs, with models having an
internally generated QBO (e.g. MRI, EMAC-L90), nudged QBO (e.g. NIES, WACCM,
SOCOLv3, EMAC-L47, EMAC-L47-o), or no QBO (e.g. CMAM, LMDZ). REF-C2 reference
simulations follow the WMO (2011) A1 scenario for ODSs and the Representative Concentration Pathway (RCP) 6.0
scenario <xref ref-type="bibr" rid="bib1.bibx49" id="paren.28"/> for other greenhouse gases, tropospheric
ozone precursors, and aerosol and aerosol precursor emissions. For
anthropogenic emissions, the CCMI recommendation was to use MACCity
<xref ref-type="bibr" rid="bib1.bibx30" id="paren.29"/> until 2000, followed by RCP 6.0 emissions.  Besides the
REF-C2 simulations we also consider the 11 sensitivity simulations with fixed
greenhouse gases (fGHGs) and with fixed ODSs (fODSs) in our analysis. These
sensitivity scenarios are both based on the REF-C2 simulation. However in the case
of the fGHG simulations, <inline-formula><mml:math id="M16" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M17" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M18" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>, and other
non-ozone-depleting GHGs are held at their 1960 value, and so we are able to
study the impact due to ODS concentration changes only (i.e. in the absence of
GHG-induced climate change). In the case of the fODS simulations the ODS
concentrations are fixed to the 1960 level throughout the simulation. All
models providing both of these sensitivity simulations are given in
Table <xref ref-type="table" rid="Ch1.T1"/>.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><?xmltex \currentcnt{1}?><label>Table 1</label><caption><p id="d1e513">Overview of the CCMI simulations, analysed for the present study. For the individual CCMs, their reference(s), their SSTs, and their available simulations (REF-C2, fGHG, fODS) are given. The numbers in brackets behind the simulations indicate the number of realizations of each REF-C2, fGHG, or fODS simulation. Detailed information about the models' SSTs and the models' representation of the QBO is given in the Supplement of <xref ref-type="bibr" rid="bib1.bibx55" id="text.30"/>.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="4">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">CCMI model</oasis:entry>
         <oasis:entry colname="col2">Reference(s)</oasis:entry>
         <oasis:entry colname="col3">SSTs</oasis:entry>
         <oasis:entry colname="col4">Analysed simulation</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">CMAM</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx41" id="text.31"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1), fGHG(1), fODS(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx75" id="text.32"/>
                  </oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">CESM1-WACCM</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx76 bib1.bibx28" id="text.33"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Interactive</oasis:entry>
         <oasis:entry colname="col4">REF-C2(4)<inline-formula><mml:math id="M21" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula>, fGHG(3), fODS(3)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx47" id="text.34"/>
                  </oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">EMAC-L90</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx39 bib1.bibx40" id="text.35"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">EMAC-L47</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx39 bib1.bibx40" id="text.36"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">EMAC-L47-o</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx39 bib1.bibx40" id="text.37"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Interactive</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1)<inline-formula><mml:math id="M22" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">GEOSCCM</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx51 bib1.bibx52" id="text.38"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx61 bib1.bibx62" id="text.39"/>
                  </oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">MRI</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx21" id="text.40"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Interactive</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx92 bib1.bibx93" id="text.41"/>
                  </oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">SOCOLv3</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx79 bib1.bibx73" id="text.42"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">NIWA-UKCA</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx53 bib1.bibx54" id="text.43"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Interactive</oasis:entry>
         <oasis:entry colname="col4">REF-C2(5), fGHG(2), fODS(2)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx80" id="text.44"/>
                  </oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">ULAQ</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx65" id="text.45"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(3), fGHG(1), fODS(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">HadGEM</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx86 bib1.bibx45" id="text.46"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Interactive</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx36 bib1.bibx53" id="text.47"/>
                  </oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx58 bib1.bibx32" id="text.48"/>
                  </oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">UMUKCA</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx53 bib1.bibx9" id="text.49"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(2)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">ACCESS-CCM</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx53 bib1.bibx54" id="text.50"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(3), fGHG(1), fODS(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx80" id="text.51"/>
                  </oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">NIES</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx37 bib1.bibx4" id="text.52"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1), fGHG(1), fODS(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">UMSLIMCAT</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx84" id="text.53"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Prescribed</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1), fGHG(1), fODS(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">CHASER</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx82" id="text.54"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Interactive</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1), fGHG(1), fODS(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">LMDz-REPROBUS</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx46 bib1.bibx83" id="text.55"/>
                  </oasis:entry>
         <oasis:entry colname="col3">interactive</oasis:entry>
         <oasis:entry colname="col4">REF-C2(1)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx25" id="text.56"/>
                  </oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">CESM1-CAM4-Chem</oasis:entry>
         <oasis:entry colname="col2">
                    <xref ref-type="bibr" rid="bib1.bibx85" id="text.57"/>
                  </oasis:entry>
         <oasis:entry colname="col3">Interactive</oasis:entry>
         <oasis:entry colname="col4">REF-C2 (3)</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><table-wrap-foot><p id="d1e519"><inline-formula><mml:math id="M19" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula> The fourth ensemble of WACCM (WACCM-4) was provided by Marta Abalos; <inline-formula><mml:math id="M20" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula> EMAC-L47 simulations are not ensembles as one simulation is with prescribed SSTs and one with interactive ocean.</p></table-wrap-foot></table-wrap>

</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>Observational data</title>
      <?pagebreak page6814?><p id="d1e1062">For observations, we make use of the BAyeSian Integrated and Consolidated
(BASIC) ozone composite that merges Stratospheric Water and Ozone Satellite Homogenized database (SWOOSH) <xref ref-type="bibr" rid="bib1.bibx20" id="paren.58"/> and Global OZone Chemistry And Related trace gas Data records
for the Stratosphere (GOZCARDS) <xref ref-type="bibr" rid="bib1.bibx27" id="paren.59"/> through the BASIC method of <xref ref-type="bibr" rid="bib1.bibx5" id="text.60"/>. The
method was developed to account for artefacts in composite datasets that are a
consequence of merging observations from different instruments that each have
unique spatial and temporal observing characteristics. As a result, these
artefacts can alias in regression analysis and bias, e.g. trend estimates
(see examples in <xref ref-type="bibr" rid="bib1.bibx5" id="altparen.61"/>). BASIC composites aim to account for and
reduce artefacts using an empirically driven Bayesian inference methodology,
but it relies on the availability of already developed ozone composites. Here,
BASIC<inline-formula><mml:math id="M23" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula> has been extended to the end of 2019 using the latest
versions of GOZCARDS, v2.20, and SWOOSH, v2.6. As such BASIC<inline-formula><mml:math id="M24" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula>
covers 1985–2019 as monthly mean zonal means on a 10<inline-formula><mml:math id="M25" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> latitude grid
from 60<inline-formula><mml:math id="M26" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–60<inline-formula><mml:math id="M27" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and over a pressure range of
147–1 <inline-formula><mml:math id="M28" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M29" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">13</mml:mn></mml:mrow></mml:math></inline-formula>–48 <inline-formula><mml:math id="M30" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula>). BASIC<inline-formula><mml:math id="M31" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula> was
presented in <xref ref-type="bibr" rid="bib1.bibx6" id="text.62"/>, and a sensitivity analysis of trends was
applied to it in <xref ref-type="bibr" rid="bib1.bibx7" id="text.63"/>, with examples of data artefacts that it
addresses in the accompanying Appendix and Supplement, respectively.</p>
      <p id="d1e1165">To obtain an observationally constrained estimate of tropical upwelling and
extratropical downwelling mass fluxes, we use the ECMWF's fifth generation of
atmospheric reanalysis data, ERA5 <xref ref-type="bibr" rid="bib1.bibx35" id="paren.64"/>. The mass fluxes are
calculated from 6-hourly data on the reduced set of pressure levels.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <label>2.3</label><title>Statistical methods</title>
      <p id="d1e1179">In some parts of our analysis, and to make a robust comparison between
multiple models and a single “real-world” realization, i.e. observations, we
form probability distributions to estimate the combined probability of the
ozone trends from all REF-C2 models. To do so, we calculate the linear trend
and the associated uncertainty using a least squares method for every
simulation. Then, to build the trend probability distribution of the models,
first 1 of the 18 CCMI models is randomly selected, assuming that the models
are randomly uniformly distributed. In case the selected CCM provided ensemble
member simulations, in a second step one of<?pagebreak page6815?> these members is randomly chosen,
thus taking into account that ensemble members are treated differently than
individual models. In the next step, the trend estimate (<inline-formula><mml:math id="M32" display="inline"><mml:mrow><mml:msup><mml:mi>t</mml:mi><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>k</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) of
the specific randomly selected CCMI model <inline-formula><mml:math id="M33" display="inline"><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> with ensemble member <inline-formula><mml:math id="M34" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula> is
calculated by randomly choosing an ozone trend value from the trends
associated and assumed normal distribution <inline-formula><mml:math id="M35" display="inline"><mml:mi mathvariant="script">N</mml:mi></mml:math></inline-formula>, which is based on
the mean <inline-formula><mml:math id="M36" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>k</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> and standard deviation <inline-formula><mml:math id="M37" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>k</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> of the
simulation's linear trend. Thus we can write the trend estimate of the selected
model simulation as <inline-formula><mml:math id="M38" display="inline"><mml:mrow><mml:msup><mml:mi>t</mml:mi><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>k</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:msup><mml:mo>=</mml:mo><mml:mi mathvariant="script">N</mml:mi><mml:mo>(</mml:mo><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>k</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:msub><mml:mo>;</mml:mo><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>k</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:msub><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>. In order to take into account the uncertainty in the
single observational dataset (<inline-formula><mml:math id="M39" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>obs</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>), we also add to the
calculated model trend estimate a random estimate of the observational noise
by taking the observational standard deviation of the linear regression
coefficient. We repeat the above-described procedure 50 000 times. With
that we have a large sample of model trends and can build up a robust
probability density function (PDF) of the REF-C2 ozone trends. From these
estimated PDFs we can then estimate the probability of a given trend relative
to the models. We derive a “probability of disagreement” between the
observational and the modelled trend distribution by taking the central
interval of the models' trend distribution with the observed trend value as
a threshold of this interval. To calculate this central interval we order the 50 000 values from the REF-C2 trend distribution according to their
probability values and then sum up the ordered probability values until the
value of the observed trend is reached. This probability value indicates our
estimate of whether the observations agree with the models; i.e. high
probability values indicate that a disagreement between models and
observations is less likely due to chance.</p>
</sec>
<sec id="Ch1.S2.SS4">
  <label>2.4</label><title>Analysis methods</title>
      <p id="d1e1345">We here provide a short description of our methodology to analyse transport
processes, which follows the studies of <xref ref-type="bibr" rid="bib1.bibx24" id="text.65"/> and
<xref ref-type="bibr" rid="bib1.bibx26" id="text.66"/>. Stratospheric mean age of air (AoA) is defined as the mean residence
time of an air parcel in the stratosphere <xref ref-type="bibr" rid="bib1.bibx31 bib1.bibx88" id="paren.67"/>. In the
CCMs, the AoA tracer is implemented as an inert tracer with a mixing ratio
that linearly increases over time as a lower boundary condition. AoA is then
calculated as the time lag between the local mixing ratio at a certain grid
point and the current mixing ratio at a reference point.</p>
      <p id="d1e1357">The residual-circulation transit time (RCTT) is the hypothetical age that air
would have if it only followed the residual circulation, thus without
processes such as eddy mixing or diffusion. RCTTs are calculated by backward
trajectories on the basis of the transformed Eulerian mean (TEM) meridional
and vertical velocities (referred to as residual velocities) with a standard
fourth-order Runge–Kutta integration <xref ref-type="bibr" rid="bib1.bibx12" id="paren.68"/>. The RCTT is then the
time that these backward trajectories require to reach the tropopause from
their respective starting point in the stratosphere. The RCTT differs from AoA
because of resolved and unresolved mixing. In the stratosphere, this is due to
the mixing of air between branches and the in-mixing of air from the
mid-latitudes into the tropical pipe, which leads to recirculation of old air
around the Brewer–Dobson Circulation (BDC) branches. In global model studies, this effect has been named
ageing by mixing (AbM) and is interpreted as the difference between AoA and
RCTT <xref ref-type="bibr" rid="bib1.bibx29" id="paren.69"><named-content content-type="pre">e.g.</named-content></xref>.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Results</title>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Ozone trends over the period 1998–2018 in CCM simulations and observations</title>
      <p id="d1e1384">In this section we analyse the ozone trends of all free-running CCMI-1
simulations (REF-C2), including all ensemble realizations of each model, for
the period 1998–2018 together with the observational data,
BASIC<inline-formula><mml:math id="M40" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula>. We chose the period 1998–2018 to be consistent with the
observational trend estimate in the ozone-recovering phase as presented by
<xref ref-type="bibr" rid="bib1.bibx6" id="text.70"/>. Note that ODSs are declining in this period as a result of
the Montreal Protocol and its amendments. By using the REF-C2 simulations we
include a wide spectrum of SST variability in the different CCMs as they use
either an interactive ocean or prescribed SSTs from a coupled ocean–atmosphere
model simulation (see Table <xref ref-type="table" rid="Ch1.T1"/>). Ozone trends are calculated by
simple linear regression using the monthly deseasonalized ozone time
series. We refrain from excluding sources of variability such as QBO, ENSO (El
Niño–Southern Oscillation), solar cycle, or volcanic eruptions in the
regression analysis to capture the full range of variability in ozone trends
over the given period. Hence our trend estimates have to be interpreted as
resulting from both forced trends (e.g. via GHG increases and ODS decreases)
and from natural and internal climate variability. In the following we
compare the calculated ozone trend from the observational data to the trends
presented in <xref ref-type="bibr" rid="bib1.bibx6 bib1.bibx7 bib1.bibx8" id="text.71"/> that used a dynamical linear
modelling (DLM) approach, which attempts to take natural sources of variability
into account. In a nutshell, DLM has many similarities with ordinary least
squares multiple linear regression (MLR), using predictor variables to account
for some of the variability in the time series (e.g. solar variability, the
QBO). Where DLM primarily differs from MLR is in allowing for a non-linear
trend to be estimated and for the seasonal cycle to evolve with time, and
therefore the shape of these terms is not predefined. For more details, see
<xref ref-type="bibr" rid="bib1.bibx44" id="text.72"/> and <xref ref-type="bibr" rid="bib1.bibx6" id="text.73"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><?xmltex \currentcnt{1}?><?xmltex \def\figurename{Figure}?><label>Figure 1</label><caption><p id="d1e1413">Latitude–pressure cross-section of the relative ozone trend over the period 1998–2018 for the observational dataset BASIC<inline-formula><mml:math id="M41" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula> and for all CCMI REF-C2 simulations. Boxes illustrate the regions selected to integrate ozone in the LS for trend comparisons later in this study, i.e. in the tropics (20<inline-formula><mml:math id="M42" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–20<inline-formula><mml:math id="M43" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S, 30–100 <inline-formula><mml:math id="M44" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>) and in the northern mid-latitudes (30–50<inline-formula><mml:math id="M45" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 30–150 <inline-formula><mml:math id="M46" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>).</p></caption>
          <?xmltex \igopts{width=469.470472pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/6811/2021/acp-21-6811-2021-f01.png"/>

        </fig>

      <?pagebreak page6817?><p id="d1e1475">The panels of Fig. <xref ref-type="fig" rid="Ch1.F1"/> show a latitude–pressure cross-section
of the ozone trend for observations (first panel of Fig. <xref ref-type="fig" rid="Ch1.F1"/>)
and all free-running CCMI model simulations. Generally, the linear trend fit
we perform on the BASIC<inline-formula><mml:math id="M47" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula> data yields similar spatial patterns and
magnitudes to those estimated in <xref ref-type="bibr" rid="bib1.bibx6" id="text.74"/> with the DLM approach (see
their Fig. 1f). There are a few small differences; e.g. our linear trend fit
results in larger positive trends in the upper stratosphere over the southern
tropics of <inline-formula><mml:math id="M48" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>, a slightly less negative trend in the Northern
Hemisphere middle stratosphere (<inline-formula><mml:math id="M49" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M50" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), and consistently large and
negative trends close to 100 <inline-formula><mml:math id="M51" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> in the tropics as opposed to a
smaller and insignificant trend at around 10<inline-formula><mml:math id="M52" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and over
100–80 <inline-formula><mml:math id="M53" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> in the DLM estimate, as shown by <xref ref-type="bibr" rid="bib1.bibx7" id="text.75"/>. Most
notably, linear-trend calculations result in small positive trends (up to
<inline-formula><mml:math id="M54" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M55" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) in the southern mid-latitude lower stratosphere as
opposed to overall negative but insignificant trends reported by
<xref ref-type="bibr" rid="bib1.bibx7" id="text.76"/> in that region. However, the comparison reveals that the
overall magnitude and trend pattern is also captured by the simple linear
regression; i.e. it is not dependent on the exact method used to calculate the
trends. Therefore, we proceed with using a linear fitting approach for the
comparison between observations and CCMs, though the above caveats should be
kept in mind when comparing with a full regression analysis using DLM
<xref ref-type="bibr" rid="bib1.bibx7" id="paren.77"/>.</p>
      <p id="d1e1581">Overall, large inter-model variability in the trends derived from the
individual REF-C2 simulations (including all ensemble members) is revealed in
Fig. <xref ref-type="fig" rid="Ch1.F1"/>. Nevertheless, a number of features can be identified
that are consistent over most models and all their ensemble members. In the
upper stratosphere (1–10 <inline-formula><mml:math id="M56" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>) nearly all simulations consistently
show an overall positive ozone trend. This ozone increase can be explained by
the decrease in ODSs <xref ref-type="bibr" rid="bib1.bibx91" id="paren.78"><named-content content-type="pre">see e.g.</named-content></xref> and by a slowdown in ozone
destruction rates as the stratosphere cools from GHG increases <xref ref-type="bibr" rid="bib1.bibx67" id="paren.79"><named-content content-type="pre">see
e.g.</named-content></xref>, as is further discussed in
Sect. <xref ref-type="sec" rid="Ch1.S3.SS5"/>. This upper-stratospheric ozone trend has been found
for climate model simulations and for observational data in several studies
before
<xref ref-type="bibr" rid="bib1.bibx77 bib1.bibx33 bib1.bibx78 bib1.bibx6 bib1.bibx8 bib1.bibx91" id="paren.80"><named-content content-type="pre">e.g.</named-content></xref>. However,
in the lower stratosphere (30–100 <inline-formula><mml:math id="M57" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> in the tropics, 150 <inline-formula><mml:math id="M58" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> in the mid-latitudes) we find a wide spread in
the ozone trends among the CCM simulations over recent decades. Many REF-C2
simulations exhibit negative trends in the tropical LS, and they are
comparable to the observational trend in magnitude and structure. In agreement
with earlier studies <xref ref-type="bibr" rid="bib1.bibx91 bib1.bibx63" id="paren.81"><named-content content-type="pre">e.g.</named-content></xref>, we show in
Sect. <xref ref-type="sec" rid="Ch1.S3.SS4"/> that this tropical ozone decrease is related to
enhanced tropical upwelling in a warmer climate. However, there are also
simulations showing a positive LS ozone trend in the tropics (i.e. GEOSCCM,
SOCOLv3, NIWA-1, WACCM-3/4, CAM4-1/2, LMDZrepro, HadGEM; note that the number
of the ensemble run is denoted with <inline-formula><mml:math id="M59" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1, <inline-formula><mml:math id="M60" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>2, and so on).  At northern and
southern mid- and high-latitudes most simulations exhibit a positive trend but with a pronounced inter-model spread. Only a few simulations show negative
trends in either northern or southern mid-latitudes (e.g. GEOSCCM, WACCM-3,
WACCM-4), but it is important to point out here that none of the 31
simulations reproduce the observed negative ozone trend pattern with an ozone
decrease covering the tropical belt and extending to the mid-latitude
(50<inline-formula><mml:math id="M61" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–50<inline-formula><mml:math id="M62" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), as shown in the upper left panel and
previously in <xref ref-type="bibr" rid="bib1.bibx6 bib1.bibx7" id="text.82"/>. This discrepancy in the LS ozone
trend between observations and models has been reported before (e.g. ozone
trends, based on CCMI simulations <xref ref-type="bibr" rid="bib1.bibx91 bib1.bibx63" id="paren.83"/>, and in
comparison to CCMVal-2 simulations <xref ref-type="bibr" rid="bib1.bibx8" id="paren.84"/>). For CCMs that provide
multiple ensemble members (WACCM, NIWA, ULAQ, ACCESS, CAM4, and UMUKCA), we
also identify a large ensemble spread in the simulated LS ozone trends. For
example in WACCM two ensemble members simulate positive tropical ozone trends,
while the two other members simulate negative tropical ozone trends. In WACCM
(as well as in NIWA and CAM4), the coupled ocean allows for differences in the
SST variability between the ensemble members, possibly explaining the large
spread in tropical ozone trends. However, as is also the case for models with
prescribed SSTs (ACCESS, ULAQ, UMUKCA) that exhibit a large spread between the
simulations, the SST variability is not the only reason for the different
trend pattern, as was similarly reported and discussed by <xref ref-type="bibr" rid="bib1.bibx8" id="text.85"/>
for CCMVal-2 models. The large spread in LS ozone trends between ensemble
members is further in agreement with the study of <xref ref-type="bibr" rid="bib1.bibx81" id="text.86"/>. They used
a nine-member ensemble of a free-running CCM simulation (CESM1-WACCM) and
showed that LS ozone trends over the years 1998–2016 are characterized by
large internal variability, with, for example, the LS ozone trend ranging from
<inline-formula><mml:math id="M63" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>6 <inline-formula><mml:math id="M64" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M65" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>6 <inline-formula><mml:math id="M66" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> per decade. But note again that none of
these ensemble members showed the coherent decrease in ozone in the tropics
and extratropics as found in observations <xref ref-type="bibr" rid="bib1.bibx8" id="paren.87"/>.</p>
      <p id="d1e1718">Following this qualitative discussion on the spread in the ozone trend pattern
between the CCM simulations, we now turn to the LS ozone trends with a more
quantitative comparison of the apparent inconsistencies between observations
and CCMs. We calculate the trends of the deseasonalized LS ozone columns for
the period 1998–2018 in two regions: the inner tropics
(20<inline-formula><mml:math id="M67" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–20<inline-formula><mml:math id="M68" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S) and in the northern mid-latitudes
(30–50<inline-formula><mml:math id="M69" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N). We choose the northern mid-latitude band
30–50<inline-formula><mml:math id="M70" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N for direct comparability with the study of
<xref ref-type="bibr" rid="bib1.bibx8" id="text.88"/>. The pressure range of the lower stratosphere was taken to
be 30–100 <inline-formula><mml:math id="M71" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> for the tropics and 30–150 <inline-formula><mml:math id="M72" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> for the
mid-latitudes to take into account the differences in latitudinal tropopause
heights. Trends and their uncertainties (represented by the 90 <inline-formula><mml:math id="M73" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>
confidence interval of the linear slope) are shown for each of the 31
available REF-C2 simulations of 18 different CCMs in Fig. <xref ref-type="fig" rid="Ch1.F2"/>. We
decided to focus on the northern mid-latitudes here because the SH
mid-latitude trends are likely more strongly influenced by the large chemical
depletion of ozone within the polar vortex. We come back to the LS ozone
trends of the southern mid-latitudes in Sect. <xref ref-type="sec" rid="Ch1.S3.SS5"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2" specific-use="star"><?xmltex \currentcnt{2}?><?xmltex \def\figurename{Figure}?><label>Figure 2</label><caption><p id="d1e1791">LS ozone trends and their uncertainties in the tropics (20<inline-formula><mml:math id="M74" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–20<inline-formula><mml:math id="M75" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S; red dots) and northern mid-latitudes (30–50<inline-formula><mml:math id="M76" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N; blue dots) together with tropical upwelling trend (black circles; for all simulations providing TEM diagnostics) for the period 1998–2018 for all REF-C2 simulations. Dashed lines separate the individual models. Moreover, observational trends (1998–2018) and multi-model mean trends are given. Observational data for ozone are taken from BASIC<inline-formula><mml:math id="M77" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula> and for tropical upwelling from ERA5 reanalysis. Error bars associated with each LS ozone trend represent the 90 <inline-formula><mml:math id="M78" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> confidence intervals. The multi-model mean trends are shown as boxplots: the solid black line in the box indicates the median, the black point indicates the MMM, and the coloured box ranges from the 25th to the 75th percentile of the trends. Crosses denote trends of individual model simulations not lying within the box.</p></caption>
          <?xmltex \igopts{width=441.017717pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/6811/2021/acp-21-6811-2021-f02.png"/>

        </fig>

      <?pagebreak page6818?><p id="d1e1844">In the tropics about half (42 <inline-formula><mml:math id="M79" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) of the REF-C2 simulations show a
significant decrease, about the same (42 <inline-formula><mml:math id="M80" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) show a non-significant
change, and about 15 <inline-formula><mml:math id="M81" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> show a significant increase in the integrated
tropical LS ozone column.  Note that significance is defined as the
non-overlap of the error bars (90 <inline-formula><mml:math id="M82" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> confidence interval) with the
zero trend. The resulting MMM ozone trend (see red bar on right of
Fig. <xref ref-type="fig" rid="Ch1.F2"/>) is negative
(<inline-formula><mml:math id="M83" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.37 <inline-formula><mml:math id="M84" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade), but it is insignificant due to the considerable spread among the
different models. The 25th–75th quantile of the distribution ranges from
<inline-formula><mml:math id="M85" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.12 to 0.20 <inline-formula><mml:math id="M86" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade (see edges of box on the right of
Fig. <xref ref-type="fig" rid="Ch1.F2"/>). Note that for the calculation of the MMM trend, we
choose to weight each of the 31 simulations equally (i.e. not taking into
account that some models have multiple ensemble members) because the trend
variations among ensemble members are as large as among the different models
over this period.</p>
      <p id="d1e1914">The observed tropical LS ozone trend of <inline-formula><mml:math id="M87" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.07 <inline-formula><mml:math id="M88" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade is
statistically significant at the 90 <inline-formula><mml:math id="M89" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> level. Thus the observed
tropical trend is more strongly negative than the MMM trend but lies within
the 90 <inline-formula><mml:math id="M90" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> confidence interval of the MMM trend
([<inline-formula><mml:math id="M91" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>1.76 <inline-formula><mml:math id="M92" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade; 1.03 <inline-formula><mml:math id="M93" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade]).</p>
      <p id="d1e1973">In the northern mid-latitudes less than half (40 <inline-formula><mml:math id="M94" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) of the REF-C2
simulations show an increase in the LS ozone column, while the remaining
60 <inline-formula><mml:math id="M95" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of the simulations show a non-significant change (either
positive or negative). There is only one simulation (WACCM-3) that shows a
significant decrease in the mid-latitude LS ozone column, and in this
simulation the tropical ozone trend is positive (but not significant). The
resulting MMM trend in the northern mid-latitudes is positive (<inline-formula><mml:math id="M96" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.63</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M97" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade) with a high inter-model spread: the 25th–75th
quantile of the distribution ranges from <inline-formula><mml:math id="M98" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.04 to
1.42 <inline-formula><mml:math id="M99" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade. Note here that the observational trend
(<inline-formula><mml:math id="M100" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.96 <inline-formula><mml:math id="M101" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade) lies outside the 90 <inline-formula><mml:math id="M102" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> confidence
interval of the MMM trend in the mid-latitudes ([<inline-formula><mml:math id="M103" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.91 <inline-formula><mml:math id="M104" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade;
2.16 <inline-formula><mml:math id="M105" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade]).</p>
      <p id="d1e2073">Figure <xref ref-type="fig" rid="Ch1.F2"/> also reveals that over the years 1998–2018 more than
half of the model simulations have a dipole trend pattern in the LS ozone
column; i.e. the sign of the tropical ozone trend is opposite to that in
mid-latitudes. This trend pattern with negative LS ozone trends in the tropics
and positive LS ozone trends in the northern mid-latitudes can be found for
almost half the simulations (45 <inline-formula><mml:math id="M106" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), and a trend pattern with a
positive ozone trend in the tropics and negative trend in the northern
mid-latitudes is found in 13 <inline-formula><mml:math id="M107" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of the simulations. The remaining
simulations do not show this dipole, but both have either a positive trend in
the tropics and the mid-latitudes (29 <inline-formula><mml:math id="M108" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) or a negative trend in both
tropics and mid-latitudes (13 <inline-formula><mml:math id="M109" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>, i.e. three simulations, namely NIWA-5,
CMAM, and WACCM-2). Only 3 out of 31 simulations simulate negative but non-significant trends both in the tropics and northern extratropics, and thus
they show a similar behaviour to observations (see right of
Fig. <xref ref-type="fig" rid="Ch1.F2"/> and <xref ref-type="bibr" rid="bib1.bibx7" id="altparen.89"/>). However, their zonal trend
patterns (see Fig. <xref ref-type="fig" rid="Ch1.F1"/>) reveal that none of these three
simulations reproduce the observed trend pattern with consistent negative
trends from 50<inline-formula><mml:math id="M110" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–50<inline-formula><mml:math id="M111" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N in the LS. Consequently it is
important to keep in mind that the results of these (averaged) trends depend
on the choice of the latitude–pressure box as the integration over a wider
latitude band can lead to a cancellation of opposing trends.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e2138">Inter-model correlation between tropical (20<inline-formula><mml:math id="M112" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–20<inline-formula><mml:math id="M113" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) and northern mid-latitude (30–50<inline-formula><mml:math id="M114" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) LS ozone column trends, calculated over the period 1998–2018  for 31 CCMI REF-C2 simulations. All ensemble members of a particular model are shown in the same colour. The observational ozone trends (BASIC<inline-formula><mml:math id="M115" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula>) are included as a star.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/6811/2021/acp-21-6811-2021-f03.png"/>

        </fig>

      <?pagebreak page6819?><p id="d1e2183">Next, we analyse whether a systematic relationship between the LS tropical and
mid-latitude trends exists in the CCM simulations. For this, the simulated
northern mid-latitude LS ozone trends are plotted against the simulated
tropical LS ozone trends over the time period 1998–2018 for all 31 REF-C2
simulations and for the observed dataset BASIC<inline-formula><mml:math id="M116" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula> in
Fig. <xref ref-type="fig" rid="Ch1.F3"/>. As discussed above, in the LS the majority
(45 <inline-formula><mml:math id="M117" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) of the models have a negative ozone trend in the tropics and a
positive trend in the northern mid-latitudes. Moreover this illustration again
highlights that the trends estimated from observational data are lying on the
outer edge of the model trend distribution. The inter-model correlation
between the tropical to mid-latitude trends is negative with a low correlation
coefficient (<inline-formula><mml:math id="M118" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.25). Thus, for the chosen period the tropical ozone trends
are only weakly linked to mid-latitude ozone trends in the models. However, we
expected that the two trends are highly (negatively) correlated as from our
understanding increased tropical upwelling leads to decreased tropical ozone,
and this upwelling increase should be linked to an increased mid-latitude
downwelling, which would enhance ozone in the mid-latitudes. However
Fig. <xref ref-type="fig" rid="Ch1.F3"/> does not support this. Also slightly varying the
period (i.e. looking at the periods 1999–2019, 2000–2020, and 2001–2021)
reveals very low negative or near-zero correlations (not shown here). To get a
better understanding of the processes leading to the given LS ozone trend
patterns, we investigate the relationship of LS ozone trends to
stratospheric transport trends in Sect. <xref ref-type="sec" rid="Ch1.S3.SS4"/>.</p>
      <p id="d1e2217">Overall we can conclude from the analysis of ozone trends in the suite of CCMI
models (see Figs. <xref ref-type="fig" rid="Ch1.F1"/>–<xref ref-type="fig" rid="Ch1.F3"/>) that the LS ozone trends exhibit a considerably
large spread across both the different models but also across ensemble
members from a single model, in particular in the mid-latitudes. This
indicates that ozone variability considerably influences the LS trends, in
agreement with the recent studies by <xref ref-type="bibr" rid="bib1.bibx18" id="text.90"/> and
<xref ref-type="bibr" rid="bib1.bibx81" id="text.91"/>. However, even when considering the high variability in
possible trends in CCM simulations, the observational trends emerge as an
unlikely realization of the simulations over the period 1998–2018. In the
next section, we analyse the robustness of this finding by varying the
period of the trend calculation and providing an in-depth statistical
analysis of the likelihood of the observed trend lying within the suite of
modelled trends.</p>
</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><title>Robustness of lower-stratospheric ozone trends</title>
      <p id="d1e2238">In the previous section we found that the observed negative ozone trend in
the LS mid-latitudes together with a simultaneous negative trend in the tropics
is unlikely, based upon the suite of CCM simulations. To further establish the
robustness of this result, we here test whether this also holds for time
periods that are slightly different to the period 1998–2018 we considered
before. Thus, in this section we first want to investigate how variability
influences the ozone trends, and second we want to quantify the likelihood of
the observed trend being a realization of the distribution of the modelled
trends. To answer those questions, we calculate the LS ozone trends by varying
the start and end years of the time period. In Fig. <xref ref-type="fig" rid="Ch1.F4"/>a and b,
the observed tropical and mid-latitude ozone trend in the LS is shown for
start years varying from 1995–2001 (<inline-formula><mml:math id="M119" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axes) and end years from 2013–2019
(<inline-formula><mml:math id="M120" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axes). Both tropical and mid-latitude LS ozone trends are
consistently negative for all chosen periods in the observations (top
row). This is in line with the results of <xref ref-type="bibr" rid="bib1.bibx7" id="text.92"/>, who found that the
observed negative sign of the tropical and mid-latitude trends remains
insensitive to changing the end year. In the tropics, observational LS ozone
trends are consistently negative, with values between <inline-formula><mml:math id="M121" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.64 and
<inline-formula><mml:math id="M122" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.24 <inline-formula><mml:math id="M123" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade for all possible start year–end year combinations. In
the mid-latitudes the trends are also negative for all shown time periods but
are more variable than in the tropics (values range between <inline-formula><mml:math id="M124" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.11 and
<inline-formula><mml:math id="M125" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.22 <inline-formula><mml:math id="M126" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade). In particular at mid-latitudes, the strongest
negative trends are found for start years of 1996 to 1998, and a sudden
decrease in the trend magnitude is found for the start years 1999 and
2000. Thus, the analysis in <xref ref-type="bibr" rid="bib1.bibx6 bib1.bibx7" id="text.93"/> and in the preceding
section focused on a period with particularly strong negative mid-latitude
ozone trends. Possible reasons for the sudden change in the trend, such as the
strong ENSO event in 1998, are discussed in Sect. <xref ref-type="sec" rid="Ch1.S4"/>. Note that
the trend magnitude increases again for the start year 2001, which again
suggests that interannual variability influences the observational
mid-latitude trends.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e2313">Tropical <bold>(a, c, e, g)</bold> and mid-latitude <bold>(b, d, f, h)</bold> LS ozone
trends (in <inline-formula><mml:math id="M127" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade) as a function of different periods for the
observational trend of BASIC<inline-formula><mml:math id="M128" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula> <bold>(a, b)</bold>, the most likely trend of the modelled REF-C2 probability distribution <bold>(c, d)</bold>, and the 1<inline-formula><mml:math id="M129" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> standard deviation (in <inline-formula><mml:math id="M130" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade) of the mean obtained from the probability distribution <bold>(e, f)</bold>. The panels <bold>(g)</bold> and <bold>(h)</bold> show the “probability of disagreement” (in per cent) between observed trends and the REF-C2 trend probability distribution. In all panels the <inline-formula><mml:math id="M131" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> coordinate denotes the different end years (2013–2019) and the <inline-formula><mml:math id="M132" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> coordinate the different start years (1995–2001).</p></caption>
          <?xmltex \igopts{width=469.470472pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/6811/2021/acp-21-6811-2021-f04.png"/>

        </fig>

      <?pagebreak page6821?><p id="d1e2391">Figure <xref ref-type="fig" rid="Ch1.F4"/>c and d display the tropical and mid-latitude trends as
a function of start and end year derived from the model simulations. To do so,
a robust estimate of the trend probability distribution considering all model
simulations was derived (see Sect. <xref ref-type="sec" rid="Ch1.S2.SS3"/>), and from this distribution
the most likely trend is shown (see peak in the models' trend probability
distributions of Figs. S1 and S2 in the Supplement).  In the tropics the ozone
trends derived from the REF-C2 simulations are negative and range from <inline-formula><mml:math id="M133" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.74</mml:mn></mml:mrow></mml:math></inline-formula>
to <inline-formula><mml:math id="M134" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M135" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade. In the mid-latitudes the trends are positive
for all possible start year–end year combinations, with values ranging from <inline-formula><mml:math id="M136" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.4</mml:mn></mml:mrow></mml:math></inline-formula>
to <inline-formula><mml:math id="M137" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1.48</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M138" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade. In contrast to the sudden change in the
mid-latitude observational trend for start years 1999 and 2000, in the REF-C2
simulations no such systematic change can be found. The estimated probability
distributions of the trends from the REF-C2 simulations (see Figs. S1 and S2)
are typically symmetric around their maximum value and show a single, central
peak. The width of the distribution changes when varying the start year–end year
combination, with narrower distributions for longer time periods. Moreover,
visual inspection of the distribution implies that the tropics (Fig. S1)
generally have Gaussian-like distributions, whereas the mid-latitudes
(Fig. S2) often show a more peaked structure, i.e. with heavier
tails. Nevertheless, as an estimate of the width of the models' trend
distribution, we show in Fig. <xref ref-type="fig" rid="Ch1.F4"/>e and f the standard deviation of
the models' distribution (in <inline-formula><mml:math id="M139" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade) in the tropics and
mid-latitudes, respectively. For longer time periods (values in lower right
corner) the standard deviation of the models' trend is smaller; i.e. the
distribution is narrower. This indicates that the influence of natural
variability is less important for longer time periods, as should be expected.</p>
      <p id="d1e2466">Given the distributions representing the combined trends of the models, we can
now quantify the disagreement between the observational trend estimate and the
models' trend probability distributions for each start year–end year
combination. In Fig. <xref ref-type="fig" rid="Ch1.F4"/>g and h the “probability of the
disagreement” between observational and modelled LS ozone trends is given for
the tropics and the mid-latitudes. The value of the “probability of
disagreement” is calculated by the central interval of the models'
probability distribution when taking the observed trend value as the threshold of
this interval. Thus, a probability value of 90 <inline-formula><mml:math id="M140" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> indicates that the
observed trend falls within the inner 90 <inline-formula><mml:math id="M141" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of the distribution; i.e.
only 10 <inline-formula><mml:math id="M142" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of the distribution is more extreme than the observed
trend: the smaller the given “probability of disagreement” value, the higher the probability that the observed trend lies within the models'
distribution. In the tropics, the observed LS ozone trend falls within the
13 <inline-formula><mml:math id="M143" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>–73 <inline-formula><mml:math id="M144" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> interval of the modelled probability
distribution; i.e. the observed trends are generally likely representations of
the models' trends. The agreement is best for short time periods (values in
diagonal in Fig. <xref ref-type="fig" rid="Ch1.F4"/>g), mostly because of the broader distribution
(see Figs. <xref ref-type="fig" rid="Ch1.F4"/>e and S1). Also for early start years (in particular
1995) and end years ranging from 2013 to 2018, the disagreement is small
because model trends are strongly negative for this period (see
Fig. <xref ref-type="fig" rid="Ch1.F4"/>c). In the mid-latitudes, the observed trend generally
lies at more distant parts of the models' trends distribution (73 <inline-formula><mml:math id="M145" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>
to 96 <inline-formula><mml:math id="M146" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>); i.e. the observed trend is a more extreme value in the
models' distribution. The disagreement is smallest for both the earlier
periods (lower left; start years 1995–1997 and end years 2013–2015) and the
later periods (upper right; start years 1999–2001 and end years
2017–2019). This coincides with the generally smaller negative trends in
those periods in observations (see Fig. <xref ref-type="fig" rid="Ch1.F4"/>b) and rather constant
trend distributions in the models (see Fig. <xref ref-type="fig" rid="Ch1.F4"/>d). For the periods
with the strongest negative observed trend (start years 1996–1998), the
observed trend lies within the central 90 <inline-formula><mml:math id="M147" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> or higher of the models'
distribution, i.e. is an unlikely representation from the modelled trends. The
sudden decrease in the observed trend magnitude for start year 1999
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>b) is reflected by a decrease in the central interval to
about 75 <inline-formula><mml:math id="M148" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>. In general, one might have expected that longer periods
lead to better agreement of the observed and modelled trend due to the smaller
influence of variability (see Fig. <xref ref-type="fig" rid="Ch1.F4"/>e and f) – as we do in the
models – however, we do not find this to be true for either the tropics or
the mid-latitudes.</p>
</sec>
<sec id="Ch1.S3.SS3">
  <label>3.3</label><title>Convergence of future lower-stratospheric ozone trends</title>
      <p id="d1e2567">In the previous section, the ozone trend robustness was analysed for time
periods of up to 25 years. We show in the following that, as the
considered time periods are extended, the influence of natural variability
decreases, and the trends converge to the trend forced by long-term GHG and ODS
concentration changes. To analyse the timing and the values of the trends'
convergence, we extend the period for the trend calculation into the future
for all REF-C2 simulations.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><?xmltex \currentcnt{5}?><?xmltex \def\figurename{Figure}?><label>Figure 5</label><caption><p id="d1e2572">Tropical (20<inline-formula><mml:math id="M149" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–20<inline-formula><mml:math id="M150" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) and northern mid-latitude (30–50<inline-formula><mml:math id="M151" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) LS ozone column trend and their uncertainties (in <inline-formula><mml:math id="M152" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade) of observations (BASIC<inline-formula><mml:math id="M153" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula>) and REF-C2 simulations as a function of the end year (red and blue dots, respectively). Tropical upwelling trends are included for all REF-C2 simulations where TEM diagnostics were available (black dots); observational tropical upwelling is taken from ERA5 reanalysis. The end year varies from 2013 to 2019 for observational data and from 2013 to 2060 for REF-C2 simulations. Error bars associated with each trend represent the 90 <inline-formula><mml:math id="M154" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> confidence intervals.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/6811/2021/acp-21-6811-2021-f05.png"/>

          <p id="d1e2633">.</p>
        </fig>

      <p id="d1e2637">Figure <xref ref-type="fig" rid="Ch1.F5"/> shows the tropical and northern mid-latitude LS
ozone trends together with the tropical upwelling trend (black)
for periods with the fixed start year 1998 and the end year varying from 2013
up to 2060 by extending the time period by steps of 1 year. For reference,
the observational trends of ozone (from BASIC<inline-formula><mml:math id="M155" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula>) and tropical
upwelling (from ERA5) are shown in the upper left panel of
Fig. <xref ref-type="fig" rid="Ch1.F5"/>, with the last available end point in the year
2019. As shown in the last section, the trends derived from observational data
are consistently negative both in the tropics and in the northern
mid-latitudes.</p>
      <?pagebreak page6823?><p id="d1e2654">As discussed in Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>, the ozone trends exhibit a strong
inter-model spread for the observational time periods. Both tropical and
mid-latitude ozone trends in the individual model simulations vary
considerably for different end point years within the observational period
(left of the vertical dashed grey lines). The northern mid-latitude trend is
generally more variable than the tropical trend. For longer time periods
extending into the future, the uncertainties in the LS ozone trends decline,
and the trends converge in all simulations. All model simulations consistently
simulate persistent negative or near-zero trends in the tropics and positive
or near-zero trends in the northern mid-latitudes. However, the timing of
convergence of the trends to this trend pattern is rather different in the
simulations, as can be inferred from Fig. <xref ref-type="fig" rid="Ch1.F5"/>; i.e. the
convergence appears to be model-dependent. For some models, the trends vary
little for end years after 2020 (e.g. MRI in Fig. <xref ref-type="fig" rid="Ch1.F5"/>),
while in other models, the trends still vary considerably until end years
around 2030 to 2040 (e.g. the four WACCM ensemble members in
Fig. <xref ref-type="fig" rid="Ch1.F5"/>). The timing of the convergence is controlled by
the ratio of the year-to-year variability to the strength of the forced
trends. The relative forcing by ODS versus GHG changes over time, and thereby
the forced ozone trends vary over the time periods as well, making it
difficult to quantify an exact date of convergence. Still, the trend estimates
for the entire period 1998 to 2060 do converge to stable values for almost all
models, thus representing the forced trend for this time period. The trend
magnitudes over this long period vary strongly between the models, from
<inline-formula><mml:math id="M156" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.10 to <inline-formula><mml:math id="M157" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.32 <inline-formula><mml:math id="M158" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade in the tropics and from <inline-formula><mml:math id="M159" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.39</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M160" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">2.00</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M161" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade in the mid-latitudes. Comparing this to the model
range of the shorter time period 1998–2040, we see that the tropical trend
(<inline-formula><mml:math id="M162" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.06</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M163" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.12 <inline-formula><mml:math id="M164" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade) has not converged to the end point
values of 2060 yet. The mid-latitude trend (<inline-formula><mml:math id="M165" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.54</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M166" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">2.15</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M167" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade) is however close to the 2060 values.</p>
      <p id="d1e2770">Overall, the mid-latitude trends converge to positive values in the majority
of the model simulations (about 85 <inline-formula><mml:math id="M168" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) by 2030. Thus, if both the
year-to-year variability and the forced response of the models is simulated
realistically, we should expect the emergence of positive mid-latitude trends
from observational records within the next decade.</p>
</sec>
<sec id="Ch1.S3.SS4">
  <label>3.4</label><title>Influence of transport processes on LS ozone trends</title>
      <p id="d1e2789">In this section we aim to improve our understanding of how transport
processes control the LS ozone trends in the models. As is well known from
earlier studies, tropical upwelling significantly influences stratospheric
ozone in the tropics <xref ref-type="bibr" rid="bib1.bibx60" id="paren.94"><named-content content-type="pre">e.g.</named-content></xref>. Enhanced tropical upwelling
leads to more transport of tropospheric ozone-poor air into the tropical
LS. Moreover, a faster removal of ozone in the tropical pipe reduces the
residence time in the LS. To analyse how tropical and mid-latitude LS ozone
trends are influenced by transport processes, we show in Fig. <xref ref-type="fig" rid="Ch1.F2"/>
the tropical upwelling trends (20<inline-formula><mml:math id="M169" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–20<inline-formula><mml:math id="M170" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S, 70 <inline-formula><mml:math id="M171" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>)
for all simulations providing TEM diagnostics. This shows that models with
strong positive tropical upwelling trends also have large negative tropical
ozone trends. However, for the mid-latitude trend it is difficult to visually
detect a clear relation with tropical upwelling trends.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><?xmltex \currentcnt{6}?><?xmltex \def\figurename{Figure}?><label>Figure 6</label><caption><p id="d1e2827">Vertical profile of the inter-model correlation coefficients for <bold>(a)</bold> tropical upwelling (20<inline-formula><mml:math id="M172" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–20<inline-formula><mml:math id="M173" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S) trends (<inline-formula><mml:math id="M174" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> per decade) to tropical (red line) and northern mid-latitude (blue line) LS ozone column trends  and for <bold>(b)</bold> mid-latitude downwelling mass flux (between the turnaround latitudes and 50<inline-formula><mml:math id="M175" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) trends (<inline-formula><mml:math id="M176" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> per decade) to tropical and northern mid-latitude LS ozone column trends. Correlations are calculated for upwelling and downwelling trends between 10 and 150 <inline-formula><mml:math id="M177" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>. Mid-latitude ozone trends are averaged over the latitude band of 30–50<inline-formula><mml:math id="M178" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N (solid blue line) and also over the dynamically defined latitude band between the turnaround latitudes to 50<inline-formula><mml:math id="M179" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N (dashed blue line). Trends are calculated over the period 1998–2018 for a subset of 20 REF-C2 simulations. Correlation coefficients which are significant on the 95 <inline-formula><mml:math id="M180" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> level are highlighted in bold.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/6811/2021/acp-21-6811-2021-f06.png"/>

        </fig>

      <p id="d1e2938">Therefore we analyse the relation of tropical upwelling and extratropical
downwelling trends to LS ozone trends in terms of a correlation
analysis. Figure <xref ref-type="fig" rid="Ch1.F6"/>a shows the inter-model correlation
between the tropical upwelling mass flux trends at different stratospheric
levels and tropical LS ozone column trends over a subset of 20 REF-C2
simulations. Additionally the correlation of the northern mid-latitude
downwelling mass flux trends at different levels and LS ozone column trends is
provided in Fig. <xref ref-type="fig" rid="Ch1.F6"/>b. As above we calculate the trends over
the period 1998–2018, and tropical ozone trends are averaged over
20<inline-formula><mml:math id="M181" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–20<inline-formula><mml:math id="M182" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and mid-latitude ozone trends over
30–50<inline-formula><mml:math id="M183" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N.</p>
      <p id="d1e2973">The correlation profiles between tropical ozone column trends and tropical
upwelling trends (red line in Fig. <xref ref-type="fig" rid="Ch1.F6"/>a) show significant
high negative correlations (<inline-formula><mml:math id="M184" display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>≈</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.8</mml:mn></mml:mrow></mml:math></inline-formula>) at all levels between 30
and 100 <inline-formula><mml:math id="M185" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>. Thus, as expected, changes in tropical upwelling at all levels
below 30 <inline-formula><mml:math id="M186" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> highly influence LS tropical ozone. This is in line with
previous studies <xref ref-type="bibr" rid="bib1.bibx60 bib1.bibx77" id="paren.95"><named-content content-type="pre">e.g.</named-content></xref>. Between 10 and
30 <inline-formula><mml:math id="M187" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>, the correlation decreases with altitude and becomes
insignificant. The correlation values of tropical ozone trends to downwelling
trends are positive and also rather high (Fig. <xref ref-type="fig" rid="Ch1.F6"/>b). This
is clear as upwelling is directly linked to downwelling; however the negative
sign of downwelling causes a sign reversal of the correlation coefficients.</p>
      <p id="d1e3024">For ozone trends in the northern mid-latitudes (30–50<inline-formula><mml:math id="M188" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), the
correlation of LS ozone to tropical upwelling trends varies in altitude from
about <inline-formula><mml:math id="M189" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.2 to <inline-formula><mml:math id="M190" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.4</mml:mn></mml:mrow></mml:math></inline-formula> (solid blue lines in Fig. <xref ref-type="fig" rid="Ch1.F6"/>a): it
is weakly negative up to 100 <inline-formula><mml:math id="M191" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>; above, the correlation turns to
positive values (<inline-formula><mml:math id="M192" display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>≈</mml:mo><mml:mn mathvariant="normal">0.4</mml:mn></mml:mrow></mml:math></inline-formula> at 70 <inline-formula><mml:math id="M193" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>). Compared to the relation
of upwelling trends to tropical ozone trends, these correlations are quite low
and not significant at the 95 <inline-formula><mml:math id="M194" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> level; moreover these correlations
are not robust when slightly varying the period (not shown). The same is
true for correlations between mid-latitude ozone trends and downwelling trends
(see solid blue lines in Fig. <xref ref-type="fig" rid="Ch1.F6"/>b). A possible reason for
the non-robust and non-significant correlations might be the choice of the
mid-latitude averaging region from 30–50<inline-formula><mml:math id="M195" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N. This region can partly
include regions of upwelling at some pressure levels, and the location of the
turnaround latitude is model-dependent. Not accounting for a dynamically
consistent averaging region might obscure the correlation analysis. Therefore,
we additionally define a dynamically more consistent mid-latitude region by
averaging the LS ozone column from the turnaround latitudes of the BDC to
50<inline-formula><mml:math id="M196" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N. For each month the averages were taken by calculating the
position of the residual stream function maximum at each level and then
averaging the LS ozone column from this turnaround latitude to
50<inline-formula><mml:math id="M197" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N. It was further ensured that tropospheric air is not included
in the averages (which could happen at levels below the tropical tropopause)
by using only the region above the tropopause.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T2" specific-use="star"><?xmltex \currentcnt{2}?><label>Table 2</label><caption><p id="d1e3125">MMM and observational ozone trends, calculated over the period 1998–2018 for tropical upwelling at 70 and 100 <inline-formula><mml:math id="M198" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>, for extratropical downwelling at 70 and 100 <inline-formula><mml:math id="M199" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>, for the LS tropical ozone column, and for the northern mid-latitude ozone column. Note that LS mid-latitude ozone trends are averaged over the fixed latitude band of 30–50<inline-formula><mml:math id="M200" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and also over the dynamically defined latitude band between the turnaround latitudes to 50<inline-formula><mml:math id="M201" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N.  MMM trends and their standard deviation are given over a subset of 20 REF-C2 simulations. Observation-based data for up- and downwelling  are taken from ERA5 reanalysis and observational data for ozone from BASIC<inline-formula><mml:math id="M202" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula>.</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">MMM</oasis:entry>
         <oasis:entry colname="col3">Observations</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Tropical upwelling trend (70 <inline-formula><mml:math id="M203" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>) [<inline-formula><mml:math id="M204" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> per decade]</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M205" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.78</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup><mml:mo>±</mml:mo><mml:mn mathvariant="normal">1.92</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M206" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.53</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Tropical upwelling trend (100 <inline-formula><mml:math id="M207" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>) [<inline-formula><mml:math id="M208" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> per decade]</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M209" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.62</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup><mml:mo>±</mml:mo><mml:mn mathvariant="normal">2.21</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M210" display="inline"><mml:mrow><mml:mn mathvariant="normal">3.14</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Downwelling trend (70 <inline-formula><mml:math id="M211" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>) [<inline-formula><mml:math id="M212" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> per decade]</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M213" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.22</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup><mml:mo>±</mml:mo><mml:mn mathvariant="normal">1.19</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M214" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.35</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Downwelling trend (100 <inline-formula><mml:math id="M215" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>) [<inline-formula><mml:math id="M216" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> per decade]</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M217" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.69</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup><mml:mo>±</mml:mo><mml:mn mathvariant="normal">2.12</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M218" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.15</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">7</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Tropical ozone trend  [<inline-formula><mml:math id="M219" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade]</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M220" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.53</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.91</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M221" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.07</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Mid-latitude (fixed) ozone trend [<inline-formula><mml:math id="M222" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade]</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M223" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.47</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.87</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M224" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.96</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Mid-latitude (dynamically) ozone trend  [<inline-formula><mml:math id="M225" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">DU</mml:mi></mml:mrow></mml:math></inline-formula> per decade]</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M226" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.78</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.91</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">–</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <?pagebreak page6824?><p id="d1e3608">The ozone trends in this dynamically defined box are slightly higher compared
to the fixed latitudinal region between 30 and 50<inline-formula><mml:math id="M227" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, but given the
large spread in trends this difference is not significant (see
Table <xref ref-type="table" rid="Ch1.T2"/>; the same is true for the longer period 1998–2040, not
shown). The correlation profiles for LS ozone trends within this dynamically
defined mid-latitude box are included in Fig. <xref ref-type="fig" rid="Ch1.F6"/>a and b
(see dashed blue line): due to the dynamical consistency of mid-latitude ozone
and the downwelling region, the correlations increase in absolute number
compared to the correlations with ozone trends in the fixed boxes, and the
correlations are more robust across different periods (not shown). In
particular, the correlation of ozone trends in the dynamically defined
averaging box to downwelling peaks at 100 <inline-formula><mml:math id="M228" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>, with a significant
correlation coefficient (<inline-formula><mml:math id="M229" display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>≈</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn></mml:mrow></mml:math></inline-formula>). Up- and downwelling at around
100 <inline-formula><mml:math id="M230" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> reflects the shallow branch of the BDC <xref ref-type="bibr" rid="bib1.bibx1 bib1.bibx24" id="paren.96"><named-content content-type="pre">see
e.g.</named-content></xref>. Thus, the significant positive
correlation of downwelling trends around this level to mid-latitude ozone
trends suggests that an enhanced shallow branch leads to a decrease in ozone
in this region. This would be consistent with enhanced horizontal advection
via the shallow branch that transports tropical ozone-poor air to the
mid-latitudes. The fact that correlations decrease to insignificant
correlation values above (and correlations to tropical upwelling even change
sign) likely reflects the relation of mid-latitude ozone trends to downward
transport of ozone via the deep branch. Thus, overall the correlation analysis
suggests that the two competing transport processes of shallow horizontal
versus deep vertical advection influence ozone in the mid-latitude LS.</p>
      <?pagebreak page6825?><p id="d1e3658">In general, the weaker correlations of mid-latitude ozone to up- and downwelling compared to tropical ozone suggest that mid-latitude ozone changes are
controlled by a variety of processes, possibly also including two-way
mixing. Furthermore, changes in not only the transport strength but also in
the background ozone gradients can lead to changes in the transport of
ozone. For example, the increase in upper-stratospheric ozone mixing ratios
could lead to enhanced downward transport of ozone despite an unchanged
downwelling strength.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><?xmltex \currentcnt{7}?><?xmltex \def\figurename{Figure}?><label>Figure 7</label><caption><p id="d1e3664">Inter-model correlation coefficients between local ozone trends and <bold>(a)</bold> local AoA trends, <bold>(b)</bold> local RCTT trends, and <bold>(c)</bold> local AbM trends. Trends are calculated over the period 1998–2018 for a subset of nine REF-C2 model simulations. White contours show the MMM ozone climatology, and the stippled regions mark where correlation coefficients are significant on the 95 <inline-formula><mml:math id="M231" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> level.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/6811/2021/acp-21-6811-2021-f07.png"/>

        </fig>

      <p id="d1e3690">To better elucidate the role of different transport processes in the different
regions, we additionally analyse the local correlation of AoA trends to the
ozone trends for a subset of nine REF-C2 simulations that provide the necessary
diagnostics (namely EMAC-L90, EMAC-L47-1, ACCESS-1, WACCM-1, CMAM, GEOS,
SOCOL, MRI, NIWA-1). As shown in Fig. <xref ref-type="fig" rid="Ch1.F7"/>a, in the
middle stratosphere the correlation coefficients are relatively weak,
consistent with the expectation that chemical processes play an important role
there. In the LS, we find very high correlations (larger than 0.8) between
ozone and AoA trends in the tropics and extending to about
40<inline-formula><mml:math id="M232" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N. Thus, inter-model differences in ozone trends are highly
controlled by differences in transport trends in this region. Negative
correlation values can be found in the LS mid-latitudes north of about
40<inline-formula><mml:math id="M233" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and above 80 to 60 <inline-formula><mml:math id="M234" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>. Interestingly, in the SH
correlations are positive throughout the LS. To analyse the role of different
transport processes, we separate AoA into the components RCTT and AbM (for details see Sect. <xref ref-type="sec" rid="Ch1.S2.SS4"/>). The
inter-model correlations between ozone trends and RCTT and AbM trends,
respectively, are shown in Fig. <xref ref-type="fig" rid="Ch1.F7"/>b and c. In the LS, RCTT trends
are highly positively correlated to ozone trends between
40<inline-formula><mml:math id="M235" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–40<inline-formula><mml:math id="M236" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, whereas for latitudes poleward of 40<inline-formula><mml:math id="M237" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>
the correlation coefficients turn to negative values. AbM trends and ozone
trends correlate strongly (and positively) in the LS for latitudes poleward of
30<inline-formula><mml:math id="M238" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>. This again underlines that in the tropical LS residual transport
changes largely control the ozone trends: negative RCTT trends (indicating
faster upwelling) are associated with negative ozone trends. This is also in
line with the findings of Fig. <xref ref-type="fig" rid="Ch1.F6"/>a. In the LS
mid-latitudes, on the other hand, both changes in residual transport (RCTTs)
and in mixing (AbM) have an impact on ozone trends, leading to the
non-homogeneous correlation structure with AoA trends
(Fig. <xref ref-type="fig" rid="Ch1.F7"/>a). In the region of our interest,
i.e. 30–50<inline-formula><mml:math id="M239" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, the different transport processes of residual
transport with its deep and shallow branch and of two-way mixing appear to
influence ozone trends: the RCTT correlations (Fig. <xref ref-type="fig" rid="Ch1.F7"/>b) suggest
that an enhancement of the meridional component of the residual circulation
(shallow branch) leads to an ozone decrease up to 40<inline-formula><mml:math id="M240" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N by enhanced
transport of tropical ozone-poor air to the mid-latitudes. This is in line with
the significant positive correlation of models' LS ozone and downwelling
trends that we presented in Fig. <xref ref-type="fig" rid="Ch1.F6"/>b. The negative
correlations between RCTT and ozone trends north of 40<inline-formula><mml:math id="M241" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N indicate
that ozone trends are driven by vertical downwelling (from the deep branch)
here: enhanced downwelling (lower transit time) is associated with transport
of ozone-rich air from above. Moreover mixing processes play a role in the
mid-latitude region. The correlation of AbM trends with ozone trends is
positive (<inline-formula><mml:math id="M242" display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>≈</mml:mo><mml:mn mathvariant="normal">0.6</mml:mn></mml:mrow></mml:math></inline-formula>) north of 30<inline-formula><mml:math id="M243" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N in the LS, indicating that
mixing is strongly influencing ozone trends in this region as well. Overall
Fig. <xref ref-type="fig" rid="Ch1.F7"/> reveals that transport processes in the LS mid-latitudes
are complex as this region is influenced by many competing transport
processes. We discuss this issue further in Sect. <xref ref-type="sec" rid="Ch1.S4"/>.</p>
</sec>
<sec id="Ch1.S3.SS5">
  <label>3.5</label><title>Forced ozone trends in models</title>
      <p id="d1e3833">In the previous sections we analysed the ozone trends of the recent 20-year
period in detail and found that modelled and observed ozone trends disagree,
especially in the northern mid-latitude LS. Assuming the observational data
are correct, the question that arises from our results is whether the
disagreement stems from the influence of natural variability or whether the
forced response to GHG or ODS concentrations is not captured correctly in the
models. Thus in the following, we investigate the relative role of GHG
versus ODS forcing in the ozone trends in the models for the observational
period and periods extending into the future. Figure <xref ref-type="fig" rid="Ch1.F8"/>a and b
show upper- and lower-stratosphere MMM ozone trends in the tropics
(20<inline-formula><mml:math id="M244" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–20<inline-formula><mml:math id="M245" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S), in the northern mid-latitudes
(30–50<inline-formula><mml:math id="M246" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), and in the southern mid-latitudes (30–50<inline-formula><mml:math id="M247" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S)
for the REF-C2 simulations as well as for the sensitivity simulations with
fixed ODS (fODS) and with fixed GHG (fGHG) concentrations (for a detailed
description of these sensitivity simulations see Sect. <xref ref-type="sec" rid="Ch1.S2.SS1"/>). These MMM
ozone trends are calculated for the recent time period (1998–2018), for a
time period which extends into the future (1998–2040), and for a future time
period (2050–2100). We also include the respective observational trends for
1998–2018. Note that for the calculation of the MMM trends only 10 model
simulations are taken into account as the fODS and fGHG simulations are not as numerous as the REF-C2 simulations (see
Table <xref ref-type="table" rid="Ch1.T1"/>). Moreover we exclude ULAQ for the MMM calculation as
its values are clear outliers compared to other models such that it would
shift the MMM to lower absolute values. Note further that the MMM ozone trends
are calculated as the average of the ensemble-means from each model. This
ensures that models are weighted equally regardless of their ensemble size, which
is desirable here as we aim to extract the forced trends, in particular for
the longer time periods.  Next to the trends averaged over the tropics and
mid-latitudes, Fig. <xref ref-type="fig" rid="Ch1.F9"/> shows the latitudinal distribution of the
ozone column trends in the upper and lower stratosphere over the period
1998–2040 for the REF-C2, fODS, and fGHG simulations. Note that we show the
trend over the period 1998–2040 here as we expect the forced signal to
emerge more clearly for this period compared to the shorter observational
period.</p>

      <?xmltex \floatpos{p}?><fig id="Ch1.F8" specific-use="star"><?xmltex \currentcnt{8}?><?xmltex \def\figurename{Figure}?><label>Figure 8</label><caption><p id="d1e3883">MMM ozone column trends in the tropics (red; 20<inline-formula><mml:math id="M248" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–20<inline-formula><mml:math id="M249" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S), in the northern mid-latitudes (blue; 30–50<inline-formula><mml:math id="M250" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), and in the southern mid-latitudes (cyan; 30–50<inline-formula><mml:math id="M251" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S) for thee different periods (i.e. 1998–2018, 1998–2040, 2050–2100) for <bold>(a)</bold> the upper stratosphere (1–10 <inline-formula><mml:math id="M252" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>) and <bold>(b)</bold> the LS (30–100 <inline-formula><mml:math id="M253" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> in the tropics, 150 <inline-formula><mml:math id="M254" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> in the mid-latitudes). The boxes extend from the lower to upper quartile of the data, with a line for the median and with whiskers to show the minimum and maximum values of the LS MMM ozone trends. MMM trends are given for REF-C2 simulations (filled boxes) as well as for fGHG and fODS simulations (not-filled boxes). Note here that for the estimate of MMM trends only 10 model simulations are taken into account as this is the maximum of available fGHG simulations, and we want to ensure that all three simulation types include the same models for the MMM trend estimate. Individual model trends are denoted by black stars for REF-C2, by black pluses for fGHG, and by black crosses for fODS. Observational data are included for the trends over the period 1998–2018 (red, blue, and cyan points, respectively).</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/6811/2021/acp-21-6811-2021-f08.png"/>

        </fig>

      <?pagebreak page6826?><p id="d1e3959"><?xmltex \hack{\newpage}?>In the upper stratosphere, the MMM ozone trends over the periods 1998–2018
and 1998–2040 are positive and of the same magnitude in tropical and
mid-latitude regions (Fig. <xref ref-type="fig" rid="Ch1.F8"/>a). The 1998–2018 MMM trends are
more than twice as strong as the observed trends (dots in
Fig. <xref ref-type="fig" rid="Ch1.F8"/>a), with only one model simulation having lower trend
values (in the tropics and NH). Even for the short period of 20 years, the
ozone trends are consistently positive for both the models and the
observations, indicating that the upper-stratosphere MMM trend is robust to
interannual variability. Therefore, this likely is the forced signal driven
by GHG and ODS changes. The analysis of the models' latitudinal distribution
in upper-stratospheric ozone column trends shows no considerable latitudinal
variation (see Fig. <xref ref-type="fig" rid="Ch1.F9"/>a). The positive upper-stratospheric MMM
trend can be explained by the combined effect of still-decreasing ODS
concentrations at the beginning of the trend periods 1998–2018 and 1998–2040
and by rising GHG concentrations causing stratospheric cooling. The
contribution of these two effects is quantified by comparing fGHG, fODS, and
REF-C2 simulations. In fGHG, the GHG-driven increase in the stratospheric
circulation (resulting mostly from the increase in SSTs) as well as GHG-induced stratospheric cooling is excluded. In fODS, the chemical ozone
destruction via ODS concentrations is excluded. Upper-stratospheric ozone
trends in fGHG and fODS are positive but considerably lower than in REF-C2,
with trends in fODS having the lowest values. This is in particular true for
the extended period 1998–2040, where we expect clearly forced trends. The
weaker upper-stratospheric ozone trend in the fGHG simulations can be
explained by the missing additional ozone increase due to GHG-induced
stratospheric cooling as ozone is photochemically controlled in these upper
regions. The weaker trend in the fODS simulations can be explained by the
missing additional increase via the recovery from ODS destruction. The
comparison of fODS and fGHG trends over the period 1998–2040 reveals that
about two-thirds of the REF-C2 upper-stratospheric trend is due to the ODS-forced
trend. The upper-stratospheric trends over the second half of the century
(2050–2100) reveal that the ceasing influence of ODS forcing manifests in
decreasing ozone trends in the fGHG simulations. However, the ODS forcing
still contributes to the ozone increase by about as much as the GHG forcing.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9" specific-use="star"><?xmltex \currentcnt{9}?><?xmltex \def\figurename{Figure}?><label>Figure 9</label><caption><p id="d1e3972">Latitudinal distribution of ozone column trends over the period 1998–2040 for all REF-C2 (grey lines), fGHG (red lines), and fODS simulations (blue lines) for <bold>(a)</bold> the upper stratosphere (1–10 <inline-formula><mml:math id="M255" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>) and <bold>(b)</bold> the LS (30–100 <inline-formula><mml:math id="M256" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>). Thick lines indicate the MMM ozone trends.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/6811/2021/acp-21-6811-2021-f09.png"/>

        </fig>

      <p id="d1e4003">For the LS, Fig. <xref ref-type="fig" rid="Ch1.F8"/>b highlights that ozone trends are highly
variable in particular for the shorter period of about 20 years and that the
MMM ozone trends over the period 1998–2018 and 1998–2040 are negative in the
tropics and positive in the mid-latitudes in the REF-C2 simulations. In
general, the mid-latitude ozone trends are very variable both in the northern
and southern mid-latitudes, but the southern mid-latitude trends are somewhat
lower (and negative in some models) for the shorter period. Also in
observations, the SH mid-latitude trend is more uncertain and variable
<xref ref-type="bibr" rid="bib1.bibx7" id="paren.97"><named-content content-type="pre">compare observational estimates in Fig. <xref ref-type="fig" rid="Ch1.F8"/>b; see also</named-content></xref>.</p>
      <p id="d1e4015">In order to attribute modelled LS ozone trends to GHG and ODS changes, we
compare the ozone trends of the REF-C2 to fGHG and fODS simulations in
Fig. <xref ref-type="fig" rid="Ch1.F9"/>b (see also MMM trends in Table S1 of the Supplement). For
the short time period of about 20 years we find that the MMM mid-latitude
ozone trends are positive and overall similar between the fGHG and the REF-C2
simulations. The fODS simulations, in contrast, show a negative MMM
mid-latitude trend but with a very high inter-model spread. Compared to the
REF-C2 simulations, the tropical LS trends are less negative in the fGHG
simulations and more negative in the fODS simulations. This is what we expect
from the missing influence of the GHG concentration rise on tropical
upwelling. But note that trends of fODS, and fGHG are not significantly
different from the REF-C2 simulation. The small, mostly non-significant
differences (not shown) with their high inter-model spread in the fGHG, fODS and
REF-C2 trends over the quite short observational period (1998–2018) again
underlines the conclusion that variability strongly impacts LS ozone trends.</p>
      <?pagebreak page6828?><p id="d1e4020">For the longer time period (1998–2040), the MMM fGHG trend in the tropical LS
is near zero (see Fig. <xref ref-type="fig" rid="Ch1.F8"/>b and Table S1). In contrast to the
trends over the short time period (1998–2018), the MMM fGHG trend can be clearly distinguished from the
negative REF-C2 trend and also from the negative MMM fODS trend, which is
comparable to the REF-C2 trend. This can be explained by the absence of
GHG-induced enhancement of tropical upwelling, which strongly influences
tropical LS ozone trends. The latitudinal distribution in Fig. <xref ref-type="fig" rid="Ch1.F9"/>b
shows in more detail the tropical LS ozone column trends in the individual
fGHG simulations (thin red lines): most models show trends near zero in the
tropical region. The slightly negative ozone trends in the tropics in two
models are a bit surprising. However, they probably can be explained by the
fact that the upper-stratospheric ozone increase can reduce the UV radiation
reaching the LS, and thus less ozone is produced there chemically <xref ref-type="bibr" rid="bib1.bibx50" id="paren.98"><named-content content-type="pre">see
e.g.</named-content></xref>. In the mid-latitudes, the MMM trend in the fGHG simulations
is positive and only slightly smaller than the REF-C2 trend, whereas the fODS
MMM trend is near zero (see Fig. <xref ref-type="fig" rid="Ch1.F8"/>b). This indicates that
enhanced downwelling associated with the strengthened circulation plays a
minor role in this selected region and is consequently not responsible for the
positive trend found in REF-C2. This weak influence of downwelling trends on
mid-latitude ozone trends is consistent with the results presented in
Sect. <xref ref-type="sec" rid="Ch1.S3.SS4"/>. There, we found that downwelling mass flux via the
deep branch and mid-latitude ozone trends are only weakly related in
REF-C2. Moreover, the near-zero ozone trend in the fODS simulations underlines
that the mid-latitude ozone trends are strongly influenced by ODS
recovery. This might be through decreased local ozone destruction (as ODSs are
still decreasing), or through ozone transport from upper or polar regions,
where ozone is increasing strongly because of the “closure of the ozone
hole”. Thus, ozone increases in the mid-latitudes, even without an enhanced
transport circulation.</p>
      <p id="d1e4036">To better understand the fact that the mid-latitude fODS trend is near zero,
although we expect transport-induced changes in the LS, we show in
Fig. <xref ref-type="fig" rid="Ch1.F9"/> (thick blue line) the latitudinal distribution of the MMM
fODS LS ozone partial-column trend. Here we see that the LS mid-latitude band
between 30–50<inline-formula><mml:math id="M257" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N lies just within a region where ozone trends are
shifting from negative to positive values. The MMM trend is negative between
30–40<inline-formula><mml:math id="M258" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and positive between 40–50<inline-formula><mml:math id="M259" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, explaining the
near-zero mid-latitude trend over the total latitude band. We suppose that the
negative trend 30–40<inline-formula><mml:math id="M260" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N can be explained by enhanced advection
through the shallow branch and/or two-way mixing and the positive trend
between 40–50<inline-formula><mml:math id="M261" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N by enhanced downwelling, as suggested by the
correlations with RCTTs (Fig. <xref ref-type="fig" rid="Ch1.F7"/>b). However, the individual models
show quite noisy behaviour in the latitudinal distribution of LS mid-latitude
ozone trends, mainly in the NH (thin blue lines in Fig. <xref ref-type="fig" rid="Ch1.F9"/>b),
indicating that the relative role of trends in the different transport
processes might differ in models. The trends in the fGHG simulations are near
zero in the inner tropics and positive at all other latitudes, indicating that
the recovery from ODSs leads to an increase in ozone almost everywhere
throughout the LS. The latitudinal distributions thus indicate that the
GHG-driven circulation changes would induce a decrease in ozone from the
tropics up to 40<inline-formula><mml:math id="M262" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and 40<inline-formula><mml:math id="M263" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S (leading to a near-zero trend in the region
30–50<inline-formula><mml:math id="M264" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), but due to the recovery of ozone from ODSs, the trend is
essentially shifted to positive values so that the average trend over
30–50<inline-formula><mml:math id="M265" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N is positive.</p>
      <p id="d1e4128">The LS ozone trends calculated over the period 2050–2100 confirm the role of
ODSs in influencing the mid-latitude ozone trends: despite a strong increase
in tropical upwelling in this period (not shown), which drives the strong
decrease in tropical ozone in the REF-C2 and likewise the fODS simulations,
mid-latitude MMM ozone trends are essentially zero (or slightly negative in
the NH) in the fGHG simulation. The effects of an ODS recovery on mid-latitude
ozone are smaller in this period due to the declining influence of ODSs, but
in the SH mid-latitudes this still leads to a robust positive ozone trend.</p>
      <p id="d1e4132">Overall our analysis of the fODS and fGHG simulations suggests that the
recovery from ODSs is a dominant player for LS mid-latitude ozone
trends. GHG-induced circulation strengthening also impacts LS mid-latitude
ozone trends,<?pagebreak page6829?> but the competing transport effects via shallow and deep
branches lead only to small transport-induced trends when averaged over the
region from 30–50<inline-formula><mml:math id="M266" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N.</p>
</sec>
</sec>
<sec id="Ch1.S4">
  <label>4</label><title>Discussion</title>
      <p id="d1e4153">In the previous sections we analysed ozone trends over periods spanning the
past 2 decades (i.e. 1998–2018) in detail. We found that modelled and
observational ozone trends agree well in the tropical lower stratosphere, but
in the northern mid-latitude LS the observed ozone trend represents an extreme
value in the distribution of model trends.</p>
      <p id="d1e4156">In the following, possible reasons for the discrepancy between the
mid-latitude ozone trends in the model simulations and the observations are discussed.  One possible reason for the disagreement between modelled and
observed LS ozone trends could be issues with the satellite records. For
example, instrument biases and drifts can lead to large uncertainties in the
observations, particularly in the lower stratosphere. The effect can manifest
as steps in the data when instruments which have different vertical
resolutions are added that can influence trend estimates. For a thorough
discussion on this topic, see
<xref ref-type="bibr" rid="bib1.bibx33" id="text.99"/>,<xref ref-type="bibr" rid="bib1.bibx5" id="text.100"/>, and <xref ref-type="bibr" rid="bib1.bibx64" id="text.101"/>. However, for the sake of
this discussion we assume that the observational data record is
correct. Hence, the question that arises from our results is whether the
disagreement stems from the influence of natural variability or whether it is
related to the forced trend, or more specifically the following can be said:
<list list-type="bullet"><list-item>
      <p id="d1e4170">The mean value of the modelled trend distributions might be incorrect. In other words, the forced trend might not be captured correctly by the models.</p></list-item><list-item>
      <p id="d1e4174">If we assume that modelled trend distributions are correct, the observed ozone trend as an unlikely representation might emerge due to very anomalous conditions during the considered periods. This may be caused by extrema in natural variability in the beginning of the time series (late 1990s) and/or in the end of the time series (late 2010s).</p></list-item><list-item>
      <p id="d1e4178">The modelled trend distribution constructed from the REF-C2 simulations might be biased because natural variability (e.g. QBO and ENSO) is not represented adequately in the models. This could lead to an overly narrow trend distribution and thus would make the observed trend seem more unlikely than it is.</p></list-item></list>
While it is not easily possible to test which of the above explanations is
correct, in the following we discuss their possible contributions to the
diagnosed disagreement in light of our results and what is known from
the literature.</p><?xmltex \hack{\newpage}?>
<sec id="Ch1.S4.SS1">
  <label>4.1</label><title>Representation of forced trends</title>
      <p id="d1e4190">Based on the CCMI-1 data, we confirmed previous studies in that the decrease
in tropical LS ozone is strongly related to the GHG-driven increase in
tropical upwelling.  The tropical upwelling trend derived from reanalysis
(ERA5) lies in the range of the upwelling trends simulated by the models but
on the upper end of the range. This is consistent with tropical ozone trends,
which are on the stronger (more negative) end of the trend range simulated by
the models as well. Circulation trends derived from reanalysis bear
considerable uncertainty <xref ref-type="bibr" rid="bib1.bibx2" id="paren.102"><named-content content-type="pre">e.g.</named-content></xref>; however reanalyses tend
to agree better in the recent decades (Thomas Birner, personal
communication, 2018, S-RIP
report). Therefore, the upwelling trend derived over the period 1998–2018
from ERA5 is likely better constrained compared to earlier periods.</p>
      <p id="d1e4198">In the mid-latitudes (30–50<inline-formula><mml:math id="M267" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), we find that the GHG-driven
circulation changes do not lead to a net trend in ozone. This is evident from
the fODS simulations (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS5"/>) and from the vanishing
mid-latitude LS ozone trends over the period 2050–2100, when the influence of
ODSs ceases. The correlation analysis in Sect. <xref ref-type="sec" rid="Ch1.S3.SS4"/> revealed
that competing processes influence ozone trends in this region: an enhanced
shallow branch in the LS can decrease ozone due to enhanced horizontal
advection, while enhanced downwelling in the deep branch increases ozone (see
correlation to RCTTs; Fig. <xref ref-type="fig" rid="Ch1.F7"/>b). In the fODS simulations, those
competing influences lead to negative LS ozone trends equatorward of 40<inline-formula><mml:math id="M268" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and 40<inline-formula><mml:math id="M269" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and to positive ozone trends poleward 40<inline-formula><mml:math id="M270" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and 40<inline-formula><mml:math id="M271" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S (see
Fig. <xref ref-type="fig" rid="Ch1.F9"/>). Thus, this leads to nearly vanishing ozone trends in the
mid-latitude region defined as 30–50<inline-formula><mml:math id="M272" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N. The consistent simulation
of positive ozone trends in the mid-latitude LS in the REF-C2 MMM for the
recent past and the coming decades is thus a result of the ODS concentration
decline rather than of GHG-driven circulation changes. The effects of
declining ODS concentrations on LS mid-latitude ozone can be related to either
the chemical recovery of ozone, leading to local increases in ozone, or maybe
more importantly to enhanced ozone transport into this region. Another effect
can be induced by the circulation changes due to ODS-driven ozone changes
that have been shown to have had a strong impact on AoA trends in the past
<xref ref-type="bibr" rid="bib1.bibx66 bib1.bibx3" id="paren.103"/>. However, future circulation changes due to
this effect are shown to be weak <xref ref-type="bibr" rid="bib1.bibx66" id="paren.104"/>. Furthermore,
ozone-induced circulation changes are stronger in the SH, not consistent with
approximately symmetric ozone trends in the mid-latitudes of both hemispheres.</p>
      <p id="d1e4271">Given that the positive mid-latitude ozone trends in models are driven by ODSs
rather than by GHG changes, the discrepancy to the observed trend could
indicate a mismatch in the relative role of the response of ozone to ODS
versus GHG forcing. This means that either the GHG-driven circulation change
in the models could be underestimated or differ in structure, or the
ODS-driven ozone increase in<?pagebreak page6830?> the mid-latitude LS could be overestimated in the
models. As for the latter, we showed that upper-stratospheric ozone increases
more strongly in the models than in the observational data (see
Fig. <xref ref-type="fig" rid="Ch1.F8"/>a). Thus, one hypothesis would be that the ODS-driven
recovery of stratospheric ozone in the period since the late 1990s is
generally overestimated in the models, which would then make negative ozone
trends in the mid-latitude LS unlikely in the models. As for the effects of
the GHG-driven circulation changes, we mentioned earlier that the MMM tropical
upwelling trend is weaker compared to the estimate from ERA5 reanalysis (see
Table <xref ref-type="table" rid="Ch1.T2"/>). However, the generally consistent tropical ozone
trends between models and observations rule out a vast underestimation of
tropical upwelling changes.  Rather, structural circulation trend differences
could contribute to the disagreement in the mid-latitudes. An indication for these structural trend differences is the lower mid-latitude downwelling trend diagnosed from ERA5, which strongly differs from the model trends (see Table <xref ref-type="table" rid="Ch1.T2"/>). This is also consistent
with the finding of poleward-shifted turnaround latitudes by <xref ref-type="bibr" rid="bib1.bibx63" id="text.105"/>,
as discussed below. While it is a likely explanation that structural
circulation trends or anomalies contribute to the observed ozone trends, it is
not easily possible to separate the role of natural variability in forming
those structural circulation trends (see discussion on natural variability
below).</p>
      <p id="d1e4283">In general, since LS mid-latitude ozone trends are driven by competing
transport processes (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS4"/>), the mismatch of trends
in this region between models and observations might also indicate a
misrepresentation of transport processes in the models. We show that ozone
trends in the LS correlate well with trends in the passive AoA tracer,
indicating that the differences in ozone trends between models are
transport-driven. While there is a long-standing discrepancy of AoA trends
derived from observations and models in the mid-stratosphere, AoA trends in
the mid-latitude LS tend to agree well between models and observations
<xref ref-type="bibr" rid="bib1.bibx91" id="paren.106"><named-content content-type="pre">see e.g. Chapter 5 of</named-content></xref>. On the other hand, climatological
mean AoA in the suite of CCMI models used in this study varies considerably
between models, and it was shown that this is due to differences in mixing
effects on AoA <xref ref-type="bibr" rid="bib1.bibx24" id="paren.107"/>.</p>
      <p id="d1e4297">The studies of <xref ref-type="bibr" rid="bib1.bibx87" id="text.108"/> and <xref ref-type="bibr" rid="bib1.bibx8" id="text.109"/> argue that the LS
mid-latitude ozone decrease in observational data is possibly linked to
enhanced two-way mixing. <xref ref-type="bibr" rid="bib1.bibx8" id="text.110"/> used effective diffusivity
<xref ref-type="bibr" rid="bib1.bibx34" id="paren.111"/> as a diagnostic for horizontal mixing and found that in
reanalysis data (JRA-55, ERA-Interim) mixing is enhanced in the 1998–2018
period. In an earlier study, <xref ref-type="bibr" rid="bib1.bibx72" id="text.112"/> also showed a substantial
increase in effective diffusivity under a changing climate for CCMs and
reanalysis data (JRA-25, ERA-40). Recently, <xref ref-type="bibr" rid="bib1.bibx63" id="text.113"/> used the TEM
budget analysis of an idealized short-lived tracer (that covaries with ozone
on interannual and decadal timescales) in 10 free-running ensemble member
simulations with the GEOSCCM model in order to identify the mechanism that is
driving the negative LS ozone trends. In contrast to the studies of
<xref ref-type="bibr" rid="bib1.bibx7" id="text.114"/> and <xref ref-type="bibr" rid="bib1.bibx87" id="text.115"/>, the study by <xref ref-type="bibr" rid="bib1.bibx63" id="text.116"/> showed
that the mixing effect is not as important for the LS mid-latitude ozone
trend. Rather they found a poleward expansion of the residual circulation in
the LS with weaker downwelling in the sub-tropics and stronger downwelling
in the mid-latitudes, leading to negative LS trends in the NH. However, as
discussed in <xref ref-type="bibr" rid="bib1.bibx63" id="text.117"/>, mixing must be considered in the context of the
specific tracer that is analysed (i.e. short-lived tracers are less sensitive
to mixing). As such, the analysis of the TEM budget for the tracer ozone could
be a focus in further investigations.</p>
      <p id="d1e4331">Overall, the LS ozone trends are strongly affected by variability over the
short period, making it difficult to infer whether the forced trends in models
and observations agree. For the models, we extended the time period into the
future to investigate the period length for which the trends converge. We find
that the inter-model spread of the ozone trends substantially diminishes for
the longer time period (1998–2040) but to a different extent for different
regions (see Fig. <xref ref-type="fig" rid="Ch1.F8"/>). In the upper stratosphere, MMM trends are
significantly positive already for the shorter period 1998–2018. In the LS,
the MMM ozone trends consistently show positive trends in the mid-latitudes
for the period 1998–2040, with a comparably low inter-model spread. Thus the
question arises as to whether we can expect observational data to also show a
positive ozone trend in the mid-latitudes in the future. If the forced model
trends are assumed to be correct, we should expect this positive trend to
emerge by about 2030 to 2040 (compare Fig. <xref ref-type="fig" rid="Ch1.F5"/>).</p>
</sec>
<sec id="Ch1.S4.SS2">
  <label>4.2</label><title>Influence of natural variability on the observed trend</title>
      <p id="d1e4347">Sources of natural variability that strongly influence LS ozone are volcanic
eruptions, the QBO, and ENSO. No major volcanic eruption occurred during the
analysed period, so we disregard this source of variability. The
influence of the QBO and ENSO on the hemispheric mean mid-latitude ozone is of
the same magnitude, and thus they can both impact LS ozone trends, as shown by
the study of <xref ref-type="bibr" rid="bib1.bibx59" id="text.118"/>.</p>
      <p id="d1e4353">We know from earlier studies that the QBO has a strong dynamical effect on the
sub-tropical and mid-latitude LS ozone <xref ref-type="bibr" rid="bib1.bibx68" id="paren.119"><named-content content-type="pre">e.g.</named-content></xref>. Moreover it
was recently shown that ozone trends in the mid-latitudes are directly linked
to the QBO as the QBO induces a secondary circulation (see
e.g. <xref ref-type="bibr" rid="bib1.bibx7" id="altparen.120"/> and Andrea Stenke, personal communication, EGU 2020). In 2016, the typical QBO phasing was
disrupted, and this has been shown to be associated with negative LS ozone
anomalies in the tropics <xref ref-type="bibr" rid="bib1.bibx43" id="paren.121"/>. These negative anomalies at the
end of the time period would lead to a strengthened negative ozone trend, and
our analysis indeed shows slightly stronger<?pagebreak page6831?> negative tropical ozone trends for
the end year 2016 compared to 2015 (see Fig. <xref ref-type="fig" rid="Ch1.F4"/>a). The
mid-latitude ozone trend is also stronger for the end year 2016, which however
does not fit expectations <xref ref-type="bibr" rid="bib1.bibx68" id="paren.122"><named-content content-type="pre">QBO-induced anomalies are of a different sign
in tropics and extratropics; see e.g.</named-content></xref>. Another way in which
the QBO could lead to decadal-scale variability in ozone and thus influence
the trends was recently reported (Jessica Neu, personal
communication, December 2018): since the QBO's
influence on tropical upwelling depends on the season, the timing of the QBO
phases is crucial for its influence on trace gas concentrations. Similarly,
<xref ref-type="bibr" rid="bib1.bibx7" id="text.123"/> pointed out that non-linear attribution may be required to
capture the QBO's impact.</p>
      <p id="d1e4378">One of the strongest warm ENSO events on record occurred in late 1997
<xref ref-type="bibr" rid="bib1.bibx38" id="paren.124"/>. By using CCM (WACCM) simulations with prescribed SSTs from
observations, <xref ref-type="bibr" rid="bib1.bibx16" id="text.125"/> showed that this strong ENSO event was
associated with low ozone values in the tropics and high values in the
mid-latitudes. This is in line with observational results by
<xref ref-type="bibr" rid="bib1.bibx70" id="text.126"/>. Consequently, mid-latitude ozone trends should be more
negative when beginning the time period with this warm ENSO year. This is
consistent with the strong mid-latitude trends in the BASIC<inline-formula><mml:math id="M273" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula>
dataset for the start year 1998 (and less so for 1996–1997; see
Fig. <xref ref-type="fig" rid="Ch1.F4"/>b). However, as the tropical trend is not associated with
weaker negative trends for the start year 1998, this explanation is again not
fully consistent.</p>
      <p id="d1e4401">As stated earlier, we have refrained from applying a multiple linear
regression (MLR), which potentially would take at least part of the named
sources of variability into account. If the trend strengths and patterns are
strongly influenced by anomalous natural-variability events, one might argue
that removing this variability via an MLR method would have a large impact on
the trends. However, the trend estimates by <xref ref-type="bibr" rid="bib1.bibx6" id="text.127"/> that take ENSO
and QBO variability into account differ only in details from the linear trend
estimates. Note that an MLR method might not fully account for the induced
signals by QBO or ENSO because, as mentioned above, their influence is likely
non-linearly dependent on the signal strength and the signal timing. Thus, an
MLR analysis cannot conclusively clarify the role of natural variability for
the observed trends.</p>
      <p id="d1e4408">Overall, the sudden systematic change in the magnitude of the mid-latitude
observational trend (Fig. <xref ref-type="fig" rid="Ch1.F4"/>b) indicates that natural variability
(in particular the strong ENSO event in 1997) influenced the observed trends
over the analysed periods and contributed to the particularly strong
disagreement of observed and modelled mid-latitude trends for the relevant time
periods.  However, the expected effects of QBO and ENSO events on the trends
are not entirely consistent between tropics and mid-latitudes. An
exceptional combination of different factors possibly led up to the particular observed
trend pattern, causing the mid-latitude trends to be more anomalous than the
tropical trends in comparison to the trend distribution derived from the
models.</p>
</sec>
<sec id="Ch1.S4.SS3">
  <label>4.3</label><title>Representation of natural variability in models</title>
      <p id="d1e4421">Above, we argued that natural variability likely influenced the observed ozone
trends, and that might partly explain that trends over the observed period
disagree with the trends in model simulations. However, how large this
disagreement is depends on the underlying trend distribution derived from the
models. For example, if the influence of natural variability is underestimated
in the models, the trend distribution is too narrow.</p>
      <p id="d1e4424">The QBO is represented differently in the individual CCMs: some models
generate a QBO internally, some models nudge winds towards a given QBO, and in
some models the representation of the QBO is missing entirely <xref ref-type="bibr" rid="bib1.bibx55" id="paren.128"><named-content content-type="pre">for more
details see</named-content></xref>. Thus, over the whole suite of models, this
could cause an underestimation of ozone variability in the models and
therewith consequently a too narrow trend distribution. Moreover, as the QBO
signal is treated differently across the REF-C2 model set-ups, we can also
expect that the inter-model differences in the QBO representation contribute
to the spread in ozone trends over recent decades.</p>
      <p id="d1e4432">The analysed free-running REF-C2 simulations use either an interactive
ocean model or SSTs from other model simulations that are coupled to an
ocean model. However, these coupled models still have biases with respect to
the simulation of ENSO <xref ref-type="bibr" rid="bib1.bibx11" id="paren.129"/>; thus ENSO-related variability in
LS ozone might also be underrepresented.</p>
      <p id="d1e4438">Further, even if the QBO and ENSO are represented with the correct signal
strength (e.g. by nudging the QBO and prescribing observed SSTs), the
induced circulation anomalies might not be captured entirely by the
models. Hence, even if hindcast simulations with prescribed observed SSTs are
used, it is not guaranteed that the effects of natural variability on ozone
trends are fully captured. It would be interesting to compare the modelled
trend distributions from the REF-C2 simulations to such hindcast simulations
(REF-C1); however, in CCMI-1 the data of those hindcast simulations are only
available until 2010. The assessment of the representation of natural
variability and its effects on ozone would require a more in-depth analysis,
which we leave for future studies.</p>
</sec>
</sec>
<sec id="Ch1.S5" sec-type="conclusions">
  <label>5</label><title>Conclusions</title>
      <p id="d1e4451">In the present study, we analysed in detail lower-stratospheric ozone trends
for the recent period 1998–2018 and variations in this period using a total
of 31 simulations of different state-of-the-art chemistry climate models and
compared them to the observation-based dataset BASIC<inline-formula><mml:math id="M274" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula>. Moreover,
we linked the ozone trends to stratospheric-circulation trends and discussed
the reasons for the differences in the LS ozone trends between models and
observations. The main findings of our study are summarized in the following.
<?xmltex \hack{\newpage}?>
<list list-type="order"><list-item>
      <p id="d1e4467">LS ozone trends over the period 1998–2018 vary strongly across different models and among different ensemble members of the same model. Therefore, internal variability strongly influences the LS ozone trends over this short time period. But even if this high variability is taken into account, none of the model simulations reproduce the
pattern of observational ozone trends with negative values extending from the southern to the northern mid-latitudes. Thus the observed LS ozone trend pattern is a rather unlikely realization in state-of-the-art CCM simulations.</p></list-item><list-item>
      <p id="d1e4471">The models' LS ozone trend (given as the most likely values of the models' trend probability distribution) remains negative in the tropics and positive in the mid-latitudes for variations in the time period between 1995 and 2019. Although there is quite a large spread in the magnitude of model trends, the trends do not show a systematic change for the different periods. For observations, LS trends remain negative in both the tropics and the mid-latitudes for all these periods. In contrast to the models' consistent trend we find a systematic shift in the trend magnitude towards less negative mid-latitude trends for the start years 1999 and 2000, which is likely associated with natural variability.</p></list-item><list-item>
      <p id="d1e4475">In the tropics, the observed trends are a likely representation by the models' trend distribution. However in the mid-latitudes the observational trends represent an extreme value of the models' probability distribution.</p></list-item><list-item>
      <p id="d1e4479">Tropical LS ozone trends are linked to the GHG-driven increase in tropical upwelling, confirming previous studies. The robust positive mid-latitude LS ozone trends simulated in the models, on the other hand, are found to be driven by changes in ODS- rather than GHG-driven circulation changes. The effects of the latter average to about zero ozone trends between 30 and 50<inline-formula><mml:math id="M275" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N because of competing processes of advection along the shallow- versus deep-circulation branch, and of two-way mixing.</p></list-item><list-item>
      <p id="d1e4492">In all models, negative trends in the tropics and positive trends in the mid-latitudes emerge for periods extending into the future (2040), but the models differ in the timing by which trends stabilize. If ozone variability and forced trends should be realistically simulated in the models, we should expect positive mid-latitude ozone trends to emerge in the next 1–2 decades from observational records, too.</p></list-item></list>
Finally we discussed the question as to whether the apparent discrepancy
between model and observational trends is due to the misrepresentation of
certain processes in the models (e.g. mixing strength, residual-circulation
strength) or due to inadequate representation of natural variability
(ENSO and QBO). Or additionally, the observational trend could just be an extreme
(but plausible) realization of the models' trend distribution. Another
hypothesis that could emerge from our results is that the discrepancy of
mid-latitude ozone trends might stem from an overestimation of ODS-induced
ozone recovery in the recent decades in models compared to observations. This
effect would be consistent with the weaker upper-stratospheric ozone trends in
the observations compared to models. However, this hypothesis needs further
investigation, as does the role of different transport processes for LS ozone
trends.</p>
</sec>

      
      </body>
    <back><notes notes-type="dataavailability"><title>Data availability</title>

      <p id="d1e4500">The CCMI-1 data used in this study can
be obtained through the British Atmospheric Data Centre (BADC) archive
(<uri>http://data.ceda.ac.uk/badc/wcrp-ccmi/data/CCMI-1/output/</uri>, <xref ref-type="bibr" rid="bib1.bibx15" id="altparen.130"/>). CESM1-WACCM data have been downloaded from
<uri>http://www.earthsystemgrid.org</uri> (<xref ref-type="bibr" rid="bib1.bibx56" id="altparen.131"/>). For instructions on access to both archives see
<uri>http://blogs.reading.ac.uk/ccmi/ccmi-1/</uri> (<xref ref-type="bibr" rid="bib1.bibx14" id="altparen.132"/>).</p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d1e4522">The supplement related to this article is available online at: <inline-supplementary-material xlink:href="https://doi.org/10.5194/acp-21-6811-2021-supplement" xlink:title="pdf">https://doi.org/10.5194/acp-21-6811-2021-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e4531">SD performed the data analysis and produced the figures. SD, RE, and HG made substantial contributions to conception and design, analysis, and interpretation of the data. WTB provided the observational ozone trends and contributed to the interpretation of the results. Moreover all authors participated in drafting the article.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e4537">The authors declare that they have no conflict of interest.</p>
  </notes><notes notes-type="sistatement"><title>Special issue statement</title>

      <p id="d1e4543">This article is part of the special issue “Chemistry–Climate Modelling Initiative (CCMI) (ACP/AMT/ESSD/GMD inter-journal SI)”. It is not associated with a conference.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e4549">We acknowledge the modelling groups for making their simulations available for
this analysis, the joint WCRP SPARC/IGAC Chemistry–Climate Model Initiative
(CCMI) for organizing and coordinating the model data analysis activity, and
the British Atmospheric Data Centre (BADC) for collecting and archiving the
CCMI model output. We thank Marta Abalos for providing us with an additional
(fourth) ensemble member of WACCM. Moreover, we want to acknowledge that the
EMAC simulations were done within the project ESCiMo (Earth System Chemistry
integrated Modelling), a national (German) contribution to the
Chemistry–Climate Model Initiative, and have been performed at the German
Climate Computing Centre DKRZ through support from the Bundesministerium für
Bildung und Forschung (BMBF).<?pagebreak page6833?> William T. Ball
was funded by the SNSF project 200020_182239
(POLE). Roland Eichinger acknowledges support
by GA CR under grant nos. 16-01562J and 18-01625S. BASIC<inline-formula><mml:math id="M276" display="inline"><mml:msub><mml:mi/><mml:mtext>SG</mml:mtext></mml:msub></mml:math></inline-formula> for
1985–2019 will be available for download from
<uri>https://data.mendeley.com/datasets/2mgx2xzzpk/4</uri> (last access: July 2020) following review of this paper.
GOZCARDS ozone data contributions from Lucien Froidevaux,
Ray Wang, John Anderson, and Ryan A. Fuller at the Jet Propulsion Laboratory are gratefully acknowledged. Last, we also thank the reviewers for their constructive comments on our manuscript.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e4566">This study was funded by the Helmholtz Association under grant VH-NG-1014 (Helmholtz-Hochschul-Nachwuchsforschergruppe MACClim).<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>
The article processing charges for this open-access <?xmltex \notforhtml{\newline}?> publication  were covered by a Research <?xmltex \notforhtml{\newline}?> Centre of the Helmholtz Association.</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e4579">This paper was edited by Paul Young and reviewed by two anonymous referees.</p>
  </notes><ref-list>
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    <!--<article-title-html>Analysis of recent lower-stratospheric ozone trends in chemistry climate models</article-title-html>
<abstract-html><p>Recent observations show a significant decrease in lower-stratospheric (LS)
ozone concentrations in tropical and mid-latitude regions since 1998. By
analysing 31 chemistry climate model (CCM) simulations performed for the
Chemistry Climate Model Initiative (CCMI; Morgenstern et al., 2017), we find
a large spread in the 1998–2018 trend patterns between different CCMs and
between different realizations performed with the same CCM. The latter in
particular indicates that natural variability strongly influences LS ozone
trends. However none of the model simulations reproduce the observed ozone
trend structure of coherent negative trends in the LS. In contrast to the
observations, most models show an LS trend pattern with negative trends in the
tropics (20°&thinsp;S–20°&thinsp;N) and positive trends in the northern
mid-latitudes (30–50°&thinsp;N) or vice versa. To investigate the influence
of natural variability on recent LS ozone trends, we analyse the
sensitivity of observational trends and the models' trend probability
distributions for varying periods with start dates from 1995 to 2001 and
end dates from 2013 to 2019. Generally, modelled and observed LS trends
remain robust for these different periods; however observational data show a
change towards weaker mid-latitude trends for certain periods, likely forced
by natural variability. Moreover we show that in the tropics the observed
trends agree well with the models' trend distribution, whereas in the
mid-latitudes the observational trend is typically an extreme value of the
models' distribution. We further investigate the LS ozone trends for extended
periods reaching into the future and find that all models develop a positive
ozone trend at mid-latitudes, and the trends converge to constant values by the
period that spans 1998–2060. Inter-model correlations between ozone trends and transport-circulation trends confirm the dominant role of
greenhouse gas (GHG)-driven tropical upwelling enhancement on the tropical LS
ozone decrease. Mid-latitude ozone, on the other hand, appears to be
influenced by multiple competing factors: an enhancement in the shallow branch
decreases ozone, while an enhancement in the deep branch increases ozone, and,
furthermore, mixing plays a role here too. Sensitivity simulations with fixed
forcing of GHGs or ozone-depleting substances (ODSs) reveal that the
GHG-driven increase in circulation strength does not lead to a net trend in LS
mid-latitude column ozone. Rather, the positive ozone trends simulated
consistently in the models in this region emerge from the decline in ODSs,
i.e. the ozone recovery. Therefore, we hypothesize that next to the influence
of natural variability, the disagreement of modelled and observed LS
mid-latitude ozone trends could indicate a mismatch in the relative role of
the response of ozone to ODS versus GHG forcing in the models.</p></abstract-html>
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