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<article xmlns:xlink="http://www.w3.org/1999/xlink" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:oasis="http://docs.oasis-open.org/ns/oasis-exchange/table" dtd-version="3.0"><?xmltex \makeatother\@nolinetrue\makeatletter?>
  <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-16-10021-2016</article-id><title-group><article-title>The representation of solar cycle signals in stratospheric ozone – Part 1: A comparison of recently updated satellite observations</article-title>
      </title-group><?xmltex \runningtitle{Solar cycle signals in stratospheric ozone -- Part~1: Satellite observations}?><?xmltex \runningauthor{A.~C.~Maycock et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1 aff2 aff6">
          <name><surname>Maycock</surname><given-names>Amanda C.</given-names></name>
          <email>a.c.maycock@leeds.ac.uk</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3 aff4">
          <name><surname>Matthes</surname><given-names>Katja</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-1801-3072</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Tegtmeier</surname><given-names>Susann</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-9206-3161</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Thiéblemont</surname><given-names>Rémi</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>Hood</surname><given-names>Lon</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-9350-8406</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Centre for Atmospheric Science, University of Cambridge, Cambridge, UK</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>National Centre for Atmospheric Science, University of Cambridge, Cambridge, UK</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>GEOMAR Helmholtz for Ocean Research, Kiel, Germany</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Christian-Albrechts Universität zu Kiel, Kiel, Germany</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>Lunar and Planetary Laboratory, University of Arizona, Tucson, Arizona, USA</institution>
        </aff>
        <aff id="aff6"><label>a</label><institution>now at: School of Earth and Environment, University of Leeds, Leeds, UK</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Amanda C. Maycock (a.c.maycock@leeds.ac.uk)</corresp></author-notes><pub-date><day>9</day><month>August</month><year>2016</year></pub-date>
      
      <volume>16</volume>
      <issue>15</issue>
      <fpage>10021</fpage><lpage>10043</lpage>
      <history>
        <date date-type="received"><day>27</day><month>October</month><year>2015</year></date>
           <date date-type="rev-request"><day>15</day><month>January</month><year>2016</year></date>
           <date date-type="rev-recd"><day>24</day><month>June</month><year>2016</year></date>
           <date date-type="accepted"><day>7</day><month>July</month><year>2016</year></date>
      </history>
      <permissions>
<license license-type="open-access">
<license-p>This work is licensed under a Creative Commons Attribution 3.0 Unported License. To view a copy of this license, visit <ext-link ext-link-type="uri" xlink:href="http://creativecommons.org/licenses/by/3.0/">http://creativecommons.org/licenses/by/3.0/</ext-link></license-p>
</license>
</permissions><self-uri xlink:href="https://acp.copernicus.org/articles/.html">This article is available from https://acp.copernicus.org/articles/.html</self-uri>
<self-uri xlink:href="https://acp.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/.pdf</self-uri>


      <abstract>
    <p>Changes in
incoming solar ultraviolet radiation over the 11-year solar cycle affect
stratospheric ozone abundances. It is important to quantify the magnitude,
structure, and seasonality of the associated solar-ozone response (SOR) to
understand the impact of the 11-year solar cycle on climate. Part 1 of this
two-part study uses multiple linear regression analysis to extract the SOR in
a number of recently updated satellite ozone datasets covering different
periods within the epoch 1970 to 2013. The annual mean SOR in the updated
version 7.0 (v7.0) Stratospheric Aerosol and Gas Experiment (SAGE) II number
density dataset (1984–2004) is very consistent with that found in the
previous v6.2. In contrast, we find a substantial decrease in the magnitude
of the SOR in the tropical upper stratosphere in the SAGE II v7.0 mixing
ratio dataset (<inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 %) compared to the v6.2 (<inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 4 %). This
difference is shown to be largely attributable to the change in the
independent stratospheric temperature dataset used to convert SAGE II ozone
number densities to mixing ratios. Since these temperature records contain
substantial uncertainties, we suggest that datasets based on SAGE II number
densities are currently most reliable for evaluating the SOR. We further
analyse three extended ozone datasets that combine SAGE II v7.0 number
densities with more recent GOMOS (Global Ozone Monitoring by Occultation of
Stars) or OSIRIS (Optical Spectrograph and Infrared Imager System)
measurements. The extended SAGE–OSIRIS dataset (1984–2013) shows a smaller
and less statistically significant SOR across much of the tropical upper
stratosphere compared to the SAGE II data alone. In contrast, the two
SAGE–GOMOS datasets (1984–2011) show SORs that are in closer agreement with
the original SAGE II data and therefore appear to provide a more reliable
estimate of the SOR. We also analyse the SOR in the recent Solar Backscatter
Ultraviolet Instrument (SBUV) Merged Ozone Dataset (SBUVMOD) version 8.6
(VN8.6) (1970–2012) and SBUV Merged Cohesive VN8.6 (1978–2012) datasets and
compare them to the previous SBUVMOD VN8.0 (1970–2009). Over their full
lengths, the three records generally agree in terms of the broad magnitude
and structure of the annual mean SOR. The main difference is that SBUVMOD
VN8.6 shows a smaller and less significant SOR in the tropical upper
stratosphere and therefore more closely resembles the SAGE II v7.0 mixing
ratio data than does the SBUV Merged Cohesive VN8.6, which has a more
continuous SOR of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 2 % in this region. The sparse spatial and
temporal sampling of limb satellite instruments prohibits the extraction of
sub-annual variations in the SOR from SAGE-based datasets. However, the
SBUVMOD VN8.6 dataset suggests substantial month-to-month variations in the
SOR, particularly in the winter extratropics, which may be important for the
proposed high-latitude dynamical response to the solar cycle. Overall, the
results highlight substantial uncertainties in the magnitude and structure of
the observed SOR from different satellite records. The implications of these
uncertainties for understanding and modelling the effects of solar
variability on climate should be explored.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p>Whilst fractional changes in total solar irradiance (TSI) between the maximum
and minimum phases of the approximately 11-year solar cycle are known to be
small (<inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 0.1 %), there is enhanced fractional variability in the
ultraviolet (UV) spectral region (<inline-formula><mml:math display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> 6 %) (e.g. <xref ref-type="bibr" rid="bib1.bibx13" id="altparen.1"/>). An
increase in UV irradiance impacts stratospheric heating rates, and thus
temperatures, through two main mechanisms: (1) enhanced absorption of
radiation by ozone and (2) enhanced production of ozone through the
photolysis of oxygen at wavelengths less than 242 nm. Consistent with these
mechanisms, past studies using observations, reanalysis data, and models have
identified an increase in annual mean temperature in the upper stratosphere
of up to <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1.5 K between solar maximum and minimum (e.g.
<xref ref-type="bibr" rid="bib1.bibx42 bib1.bibx39 bib1.bibx1" id="altparen.2"/>) and an increase in ozone abundances
of a few percent <xref ref-type="bibr" rid="bib1.bibx49 bib1.bibx19" id="paren.3"/>. These radiatively driven changes
modify the meridional temperature gradients in the upper stratosphere, which
can lead to a modulation of planetary wave propagation and breaking and
changes in the strength of the stratospheric polar vortex (e.g.
<xref ref-type="bibr" rid="bib1.bibx29 bib1.bibx33 bib1.bibx34 bib1.bibx18 bib1.bibx26" id="altparen.4"/>). Such feedback
mechanisms can lead to amplified changes in regional surface climate via
stratosphere–troposphere dynamical coupling (e.g. <xref ref-type="bibr" rid="bib1.bibx18" id="altparen.5"/>).
Constraining the stratospheric response to solar forcing is therefore
important for understanding solar–climate coupling and potential sources of
decadal variability in the climate system (e.g. <xref ref-type="bibr" rid="bib1.bibx51" id="altparen.6"/>).</p>
      <p>The solar-ozone response (SOR) has been estimated to make a substantial
contribution to variations in stratospheric temperatures over the 11-year
solar cycle. <xref ref-type="bibr" rid="bib1.bibx17" id="text.7"/> used an estimate of the SOR from SAGE II
(Stratospheric Aerosol and Gas Experiment II) version 6.2 (v6.2) satellite
ozone mixing ratio data and spectral solar irradiance (SSI) variations from
<xref ref-type="bibr" rid="bib1.bibx31" id="text.8"/> to show that the contribution of the SOR to temperature changes
between the maximum and minimum phases of the 11-year solar cycle is around
60 % at the tropical stratopause, 30–40 % between 40 and 50 km, and
70–80 % between 20 and 30 km. <xref ref-type="bibr" rid="bib1.bibx47" id="text.9"/> conducted similar
calculations using estimates of the SOR from two atmospheric chemical models
and found that the SOR accounted for only around 20–25 % of the solar
cycle temperature response near the tropical stratopause. Since the two
studies used similar SSI datasets, this difference must arise from the SOR
estimated from SAGE II observations used by <xref ref-type="bibr" rid="bib1.bibx17" id="text.10"/> being different
from that simulated in the atmospheric chemistry models used by
<xref ref-type="bibr" rid="bib1.bibx47" id="text.11"/>. It is therefore important to evaluate the SOR and its
uncertainties in different observational datasets to understand the climate
response to solar variability and to provide an
independent means for evaluating the performance of atmospheric chemistry
models (e.g. <xref ref-type="bibr" rid="bib1.bibx1" id="altparen.12"/>; see also Part 2, Maycock et al., 2016).</p>
      <p>Whilst past studies have quantified the SOR in observations (e.g.
<xref ref-type="bibr" rid="bib1.bibx49 bib1.bibx43 bib1.bibx45 bib1.bibx46 bib1.bibx5 bib1.bibx32" id="altparen.13"/>), there are
differences in the magnitudes and structures between individual satellite
records. It is not clear whether these are due to inter-instrument
differences in observational periods and/or differences in instrument
resolution, sampling, or drifts. There are also apparent differences in the
structure and magnitude of the SOR between observations and atmospheric
chemistry models (e.g. <xref ref-type="bibr" rid="bib1.bibx19 bib1.bibx49 bib1.bibx1 bib1.bibx11" id="altparen.14"/>). These
issues are compounded by current uncertainties in the characteristics of
SSI variability (e.g. <xref ref-type="bibr" rid="bib1.bibx13" id="altparen.15"/>), which have
implications for constraining the magnitude and structure of the SOR because
of its dependence on photochemical processes <xref ref-type="bibr" rid="bib1.bibx20 bib1.bibx12 bib1.bibx2" id="paren.16"/>.
These factors present an additional challenge for understanding and
evaluating the overall climate response to solar variability, particularly
since dynamical feedbacks may amplify the effects of an initially small
forcing (e.g. <xref ref-type="bibr" rid="bib1.bibx34 bib1.bibx27" id="altparen.17"/>).</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><caption><p>Overview of the satellite ozone datasets used in this study.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="5">
     <oasis:colspec colnum="1" colname="col1" align="justify" colwidth="91.048819pt"/>
     <oasis:colspec colnum="2" colname="col2" align="justify" colwidth="102.429921pt"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:colspec colnum="5" colname="col5" align="justify" colwidth="85.358268pt"/>
     <oasis:thead>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Dataset</oasis:entry>  
         <oasis:entry colname="col2">Type</oasis:entry>  
         <oasis:entry colname="col3">Time period</oasis:entry>  
         <oasis:entry colname="col4">Units</oasis:entry>  
         <oasis:entry colname="col5">Reference</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">SAGE II v6.2</oasis:entry>  
         <oasis:entry colname="col2">Raw satellite product: solar <?xmltex \hack{\hfill\break}?>occultation instrument</oasis:entry>  
         <oasis:entry colname="col3">1984–2004</oasis:entry>  
         <oasis:entry colname="col4">ppmv; cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">
                    <xref ref-type="bibr" rid="bib1.bibx54" id="text.18"/>
                  </oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SAGE II v7.0</oasis:entry>  
         <oasis:entry colname="col2">Raw satellite product: solar <?xmltex \hack{\hfill\break}?>occultation instrument</oasis:entry>  
         <oasis:entry colname="col3">1984–2004</oasis:entry>  
         <oasis:entry colname="col4">ppmv; cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">
                    <xref ref-type="bibr" rid="bib1.bibx8" id="text.19"/>
                  </oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SAGE–GOMOS 1</oasis:entry>  
         <oasis:entry colname="col2">Combined satellite product, <?xmltex \hack{\hfill\break}?>including SAGE II v7.0</oasis:entry>  
         <oasis:entry colname="col3">1984–2011</oasis:entry>  
         <oasis:entry colname="col4">cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">
                    <xref ref-type="bibr" rid="bib1.bibx30" id="text.20"/>
                  </oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SAGE–GOMOS 2</oasis:entry>  
         <oasis:entry colname="col2">Combined satellite product, <?xmltex \hack{\hfill\break}?>including SAGE II v7.0</oasis:entry>  
         <oasis:entry colname="col3">1984–2011</oasis:entry>  
         <oasis:entry colname="col4">cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">
                    <xref ref-type="bibr" rid="bib1.bibx41" id="text.21"/>
                  </oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">SAGE–OSIRIS</oasis:entry>  
         <oasis:entry colname="col2">Combined satellite product, <?xmltex \hack{\hfill\break}?>including SAGE II v7.0</oasis:entry>  
         <oasis:entry colname="col3">1984–2013</oasis:entry>  
         <oasis:entry colname="col4">cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">
                    <xref ref-type="bibr" rid="bib1.bibx5" id="text.22"/>
                  </oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SBUVMOD VN8.0</oasis:entry>  
         <oasis:entry colname="col2">Raw satellite product: <?xmltex \hack{\hfill\break}?>nadir-viewing instrument</oasis:entry>  
         <oasis:entry colname="col3">1970–2009</oasis:entry>  
         <oasis:entry colname="col4">ppmv</oasis:entry>  
         <oasis:entry colname="col5"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SBUVMOD VN8.6</oasis:entry>  
         <oasis:entry colname="col2">Raw satellite product: <?xmltex \hack{\hfill\break}?>nadir-viewing instrument</oasis:entry>  
         <oasis:entry colname="col3">1970–2012</oasis:entry>  
         <oasis:entry colname="col4">ppmv</oasis:entry>  
         <oasis:entry colname="col5">
                    <xref ref-type="bibr" rid="bib1.bibx38 bib1.bibx15" id="text.23"/>
                  </oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SBUV Merged Cohesive <?xmltex \hack{\hfill\break}?>VN8.6</oasis:entry>  
         <oasis:entry colname="col2">Raw satellite product: <?xmltex \hack{\hfill\break}?>nadir-viewing instrument</oasis:entry>  
         <oasis:entry colname="col3">1978–2012</oasis:entry>  
         <oasis:entry colname="col4">ppmv</oasis:entry>  
         <oasis:entry colname="col5">
                    <xref ref-type="bibr" rid="bib1.bibx55" id="text.24"/>
                  </oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p>The aim of this two-part study (see also Maycock et al., 2016) is to evaluate
the representation of the SOR and its uncertainties in satellite observations
and global models. The present Part 1 describes the SOR in the latest
version 7.0 (v7.0) of the SAGE II dataset and compares it to the former v6.2,
which has been used in several solar-climate studies (e.g.
<xref ref-type="bibr" rid="bib1.bibx49 bib1.bibx17" id="altparen.25"/>) as well as in several ozone databases developed for climate
models without interactive chemistry <xref ref-type="bibr" rid="bib1.bibx7 bib1.bibx4" id="paren.26"/>. A number of
merged satellite ozone datasets, which extend SAGE II using more recent
measurements, have also been created and analysed as part of the WCRP/SPARC
(World Climate research Programme/Stratosphere-troposphere Processes and
their Role in Climate) SI<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>N ozone trends activity (e.g. <xref ref-type="bibr" rid="bib1.bibx53" id="altparen.27"/>);
we analyse the SOR in three of these combined satellite ozone datasets. We
also analyse the SOR in two versions of the recently released version 8.6 (VN8.6) of the
Solar Backscatter Ultraviolet Instrument (SBUV) data and compare these to the
former SBUV Merged Ozone Dataset (SBUVMOD) VN8.0 data.</p>
      <p>Part 2 of the study (Maycock et al., 2016) describes the SOR in chemistry–climate model simulations from the WCRP/SPARC Chemistry-Climate
Model Initiative (CCMI) and compares them to a subset of the observational
records discussed here that are determined to be most reliable for diagnosing
the SOR (see below). Part 2 also discusses the representation of the SOR in
the climate model ozone dataset created for the fifth Coupled Model
Intercomparison Project (CMIP5) <xref ref-type="bibr" rid="bib1.bibx7" id="paren.28"/>. This leads to a discussion of
the representation of the SOR in the ozone dataset being created for CMIP6 (Hegglin et al., 2016).</p>
      <p>Given the potential application of the results described here for use in
climate model simulations, it is prudent to briefly review the typical
requirements of an ozone database for models by describing the CMIP5 dataset
as a representative example <xref ref-type="bibr" rid="bib1.bibx7" id="paren.29"/> (see also <xref ref-type="bibr" rid="bib1.bibx4" id="altparen.30"/>). The
CMIP5 ozone database provided monthly mean ozone mixing ratios on a regular
latitude–pressure grid at a horizontal resolution of
5<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 5<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> (long <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> lat) on
24 pressure levels covering 1000–1 hPa for the period 1850–2100. Data were
provided on the following pressure levels: 1000, 850, 700, 600, 500, 400,
300, 250, 200, 150, 100, 80, 70, 50, 30, 20, 15, 10, 7, 5, 3, 2, 1.5, and
1 hPa. Stratospheric ozone data (at <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>p</mml:mi><mml:mo>≤</mml:mo><mml:mn>300</mml:mn></mml:mrow></mml:math></inline-formula> hPa) were given as zonal
mean values. Therefore, any description of the SOR must fulfil these (or
similar) criteria to be viable for use in climate models (i.e. global
coverage at monthly mean resolution and with sufficient vertical and
horizontal resolution throughout the stratosphere).</p>
</sec>
<sec id="Ch1.S2">
  <title>Ozone datasets</title>
      <p>The satellite ozone datasets examined in this study are
summarized in Table 1. A detailed overview of their spatial and temporal
sampling characteristics and, where appropriate, their merging procedures is
provided by <xref ref-type="bibr" rid="bib1.bibx53" id="text.31"/> and references therein. Their main properties are
briefly summarized below. Since our goal is to extract a signal with power on quasi-decadal timescales, it is desirable to use the longest available
time series, and we therefore analyse all datasets over their full periods.
For the longest record considered, this amounts to approximately three solar
cycles.</p>
<sec id="Ch1.S2.SS1">
  <title>SAGE II-based records</title>
      <p>The SAGE II record forms the basis of many long-term ozone datasets (see,
e.g., <xref ref-type="bibr" rid="bib1.bibx53" id="altparen.32"/>). As a limb-viewing instrument, the spatial and temporal
sampling of SAGE is fairly sparse, with a given latitude measured
approximately once per month; however, it is recognized as having good
long-term stability and a vertical resolution of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 km in the
stratosphere, which are characteristics that are likely to be important for
analysing the SOR. We use zonal and monthly mean ozone data from October 1984
to August 2005 provided through the WCRP/SPARC Data Initiative (SDI)
<xref ref-type="bibr" rid="bib1.bibx50" id="paren.33"/>.</p>
      <p>The native retrieval coordinate of SAGE II is units of ozone number densities
on altitude levels; data are post-processed to volume mixing ratios (vmr) on
pressure levels using temperatures from a meteorological reanalysis dataset.
The SAGE II retrieval algorithm was recently updated as part of the version 7.0 release <xref ref-type="bibr" rid="bib1.bibx8" id="paren.34"/>. The SOR in SAGE II v6.2 data has been discussed
in a number of studies: e.g. <xref ref-type="bibr" rid="bib1.bibx43" id="text.35"/>, <xref ref-type="bibr" rid="bib1.bibx49" id="text.36"/>, and <xref ref-type="bibr" rid="bib1.bibx17" id="text.37"/> for mixing
ratios and <xref ref-type="bibr" rid="bib1.bibx45" id="text.38"/> for number densities. Here we compare the SOR
in the latest v7.0 release to the previous v6.2 in units of number densities
and mixing ratios. It is important to conduct this comparison in both sets
of coordinates because the temperature record used to convert SAGE II to mixing
ratios was changed between v6.2 and v7.0 from National Meteorological
Center/National Center for Environmental Prediction (NMC/NCEP) data to Modern
Era-Retrospective Analysis for Research and Applications version 1 (MERRA-1)
reanalysis data. The impact of this change on the SOR in SAGE II datasets has not been previously
evaluated and is described in Sect. <xref ref-type="sec" rid="Ch1.S4.SS1"/>.</p>
      <p>As a solar occultation instrument, SAGE II profiles can be categorized as a
sunrise (SR) or sunset (SS) measurement. There are known variations in the
relative number of SR/SS profiles over the SAGE II record. For example,
SAGE II obtained profiles in two narrow latitude bands each day, 15 each at
sunrise and sunset, but after November 2000 SAGE II measured only one profile
per orbit at either SR or SS. These variations in SR/SS sampling have been
shown to affect estimates of climatological ozone values due to diurnal cycle
effects <xref ref-type="bibr" rid="bib1.bibx52" id="paren.39"/> but could also
affect temporal variability in monthly mean ozone values. To account for the
possible effects of these sampling issues on the estimation of the SOR, we
add an additional term to the multiple linear regression model for SAGE II
data that represents the fraction of SR to total (SR <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> SS) profiles used
to generate each monthly mean data point (see Sect. <xref ref-type="sec" rid="Ch1.S3"/>).</p>
      <p>The SAGE II mission stopped measuring in 2005. Since then several satellite
instruments have continued to measure ozone, and there are now a number of
combined datasets that have extended SAGE II to near the present day. These
datasets were recently analysed as part of the WCRP/SPARC SI<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>N activity
to evaluate long-term ozone trends (see <xref ref-type="bibr" rid="bib1.bibx53" id="altparen.40"/>, and references
therein) and include SWOOSH (Stratospheric Water and OzOne Satellite
Homogenized) <xref ref-type="bibr" rid="bib1.bibx9" id="paren.41"/>, GOZCARDS (Global OZone Chemistry And Related trace gas
Data records for the Stratosphere) <xref ref-type="bibr" rid="bib1.bibx16" id="paren.42"/>, SAGE–GOMOS (Global
Ozone Monitoring by Occultation of Stars) <xref ref-type="bibr" rid="bib1.bibx30 bib1.bibx41" id="paren.43"/>, and
SAGE–OSIRIS (Optical Spectrograph and Infrared Imager System)
<xref ref-type="bibr" rid="bib1.bibx5" id="paren.44"/>. As mentioned above, SAGE II mixing ratios are produced by
the conversion of number densities using an independent temperature record. The
uncertainties in the SOR that result from using different stratospheric
temperature records for this conversion are demonstrated in Sect. <xref ref-type="sec" rid="Ch1.S4.SS1"/>.
This leads us to focus our analysis of the SOR on the extended SAGE II records that
provide ozone as number densities and are therefore less dependent on the
conversion issues that accompany the choice of a particular temperature
record (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS2"/>). Since SWOOSH and GOZCARDS currently only
provide ozone mixing ratios, we do not analyse them here.</p>
      <p>The three extended ozone datasets all include SAGE II v7.0 number densities.
Differences in the SOR between the datasets may therefore arise as a result
of the more recent measurements used to extend SAGE II and/or from the
methods used to merge the different satellite records. Two of the datasets
extend SAGE II using GOMOS, which flew on the ENVISAT satellite and covers
2002–2011, but take different approaches for combining the two records.
<xref ref-type="bibr" rid="bib1.bibx30" id="text.45"/> use GOMOS as a reference and adjust SAGE II sunrise and sunset
profiles separately at each latitude and altitude; this dataset will be
referred to as SAGE–GOMOS 1. Conversely, <xref ref-type="bibr" rid="bib1.bibx41" id="text.46"/> use SAGE II as a
reference and adjust GOMOS data using seasonally varying offsets at each
latitude and altitude; this dataset will be referred to as SAGE–GOMOS 2. The
third dataset analysed extends SAGE II using OSIRIS data and covers 1984–2013
<xref ref-type="bibr" rid="bib1.bibx5 bib1.bibx48" id="paren.47"/>. Latitude- and altitude-dependent offsets are
calculated for the deseasonalized data during the instrument overlap period
(January 2002–August 2005), and the OSIRIS data are adjusted to produce a
consistent combined SAGE II and OSIRIS time series.</p>
</sec>
<sec id="Ch1.S2.SS2">
  <title>SBUV-based records</title>
      <p>In addition to SAGE II, the other main long-term internally calibrated
satellite ozone dataset is comprised of data from the Backscatter Ultraviolet
Radiometer (BUV) and Solar Backscatter Ultraviolet Radiometer (SBUV)
instruments on board Nimbus satellites and the SBUV/2 instruments on various
National Oceanic and Atmospheric Administration (NOAA) satellites. Data are
available as mixing ratios on pressure levels from January 1970 to near the
present day. As nadir-viewing instruments, the BUV/SBUV records have more
frequent global coverage than the limb-viewing SAGE II, but their vertical
resolution is at least 1 order of magnitude poorer at pressures greater than
<inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 15 hPa, rendering it more difficult to resolve detailed ozone
structures in the mid and lower stratosphere. Since the entire BUV/SBUV
record is comprised of multiple records from different satellites,
inter-instrument biases and drifts must also be accounted for to produce a
homogenized record.</p>
      <p>We analyse zonal and monthly mean data from SBUVMOD VN8.0 and the latest release SBUV VN8.6
<xref ref-type="bibr" rid="bib1.bibx38 bib1.bibx3" id="paren.48"/>, thereby complementing previous analyses of the SOR
(e.g. <xref ref-type="bibr" rid="bib1.bibx49" id="altparen.49"/>). SBUVMOD VN8.0 covers the period 1970–2009 and was
downloaded from <uri>http://acd-ext.gsfc.nasa.gov/Data_services/merged/data/sbuv.70-09.za.v8_prof.vmr.rev1.txt</uri>.</p>
      <p>Two versions of the SBUV VN8.6 record have been produced so far: the
SBUVMOD VN8.6 dataset from NASA, which covers 1970–2012 <xref ref-type="bibr" rid="bib1.bibx15" id="paren.50"/>, and the
SBUV Merged Cohesive dataset from NOAA, which covers 1978–2012 <xref ref-type="bibr" rid="bib1.bibx55" id="paren.51"/>.
These are identical to the datasets analysed as part of the SI<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>N
activity (e.g. <xref ref-type="bibr" rid="bib1.bibx53" id="altparen.52"/>). The two SBUV VN8.6 datasets contain some
differences in the data that are included from different instruments within a
particular period (see Fig. 1 in <xref ref-type="bibr" rid="bib1.bibx53" id="altparen.53"/>) and in the methods for
averaging and merging these data. SBUV Merged Cohesive VN8.6 uses data from a
single instrument in any time period; the individual records are then
bias-corrected to produce a continuous record <xref ref-type="bibr" rid="bib1.bibx55" id="paren.54"/>. In contrast,
SBUVMOD VN8.6 is constructed by averaging all available data within a
particular time window <xref ref-type="bibr" rid="bib1.bibx15" id="paren.55"/>. The SBUVMOD datasets extend back to
1970 by including data from the BUV instrument on Nimbus 4 from 1970 to 1976,
whereas the SBUV Merged Cohesive dataset starts from 1978 with the first SBUV
instrument on Nimbus 7.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <title>The multiple linear regression model</title>
      <p>Following numerous earlier studies (e.g.
<xref ref-type="bibr" rid="bib1.bibx14 bib1.bibx49 bib1.bibx39" id="altparen.56"/>), the SOR is diagnosed using multiple
linear regression (MLR); this technique enables the signals associated with
different forcings within a single time series to be separated.</p>
      <p>The ozone data are first deseasonalized by removing the long-term monthly
mean at each latitude and pressure (or altitude). As in past studies, we then
perform an MLR analysis on the time series of monthly mean ozone anomalies at
each location, O<inline-formula><mml:math display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn><mml:mo>′</mml:mo></mml:msubsup><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, to diagnose the 11-year solar cycle component:

              <disp-formula specific-use="align" content-type="numbered"><mml:math display="block"><mml:mtable displaystyle="true"><mml:mtr><mml:mtd><mml:mrow><mml:msubsup><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi></mml:mrow><mml:mn mathvariant="normal">3</mml:mn><mml:mo>′</mml:mo></mml:msubsup><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>=</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mi>A</mml:mi><mml:mo>×</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">F</mml:mi><mml:mn>10.7</mml:mn></mml:mrow><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mi>B</mml:mi><mml:mo>×</mml:mo><mml:msub><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mi>C</mml:mi><mml:mo>×</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">EESC</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>+</mml:mo><mml:mi>D</mml:mi><mml:mo>×</mml:mo><mml:mi mathvariant="normal">ENSO</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mi>E</mml:mi><mml:mo>×</mml:mo><mml:msub><mml:mi mathvariant="normal">QBO</mml:mi><mml:mi>A</mml:mi></mml:msub><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mi>F</mml:mi></mml:mrow></mml:mtd></mml:mtr><mml:mlabeledtr id="Ch1.E1"><mml:mtd/><mml:mtd/><mml:mtd><mml:mrow><mml:mo>×</mml:mo><mml:msub><mml:mi mathvariant="normal">QBO</mml:mi><mml:mi>B</mml:mi></mml:msub><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mi>r</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

          where <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> is a residual. The analysis mainly focuses on annual-mean
signals, which are calculated by regressing all months as a single
time series.</p>
      <p>The monthly basis functions are the F10.7 cm radio solar flux
(<uri>http://lasp.colorado.edu/lisird/tss/noaa_radio_flux.html</uri>), the CO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>
concentration at Mauna Loa (<uri>http://www.esrl.noaa.gov/gmd/ccgg/trends/data.html</uri>), the equivalent
effective stratospheric chlorine (EESC), the Nino 3.4 index calculated from
the Extended Reconstructed Sea Surface Temperature (ERSST) v3b dataset
(<uri>http://www.esrl.noaa.gov/psd/data/gridded/data.noaa.ersst.html</uri>),
and two quasi biennial oscillation (QBO) indices representing tropical zonal
winds at 30 and 50 hPa (<uri>http://www.cpc.ncep.noaa.gov/data/indices/</uri>). Figure <xref ref-type="fig" rid="Ch1.F1"/> shows example
time series of these indices from 1970 to 2015 in arbitrary units. The
coefficients <inline-formula><mml:math display="inline"><mml:mi>A</mml:mi></mml:math></inline-formula>–<inline-formula><mml:math display="inline"><mml:mi>F</mml:mi></mml:math></inline-formula> are calculated using linear least squares regression.</p>
      <p>The El Niño–Southern Oscillation (ENSO) is the main regressor for which
a lagged response in stratospheric ozone might be expected; however, we find
that the SOR is not sensitive to lagging the ozone anomalies with respect to
the Nino 3.4 index by 0–12 months. We therefore do not include any lags in
Eq. (<xref ref-type="disp-formula" rid="Ch1.E1"/>). We have also tested the sensitivity of the diagnosed SOR
to the use of a spatially varying EESC field using
output from the UM-UKCA chemistry–climate model REF-C1 CCMI integration.
However, this has virtually no effect on the SOR compared to the use of a
single EESC time series for all locations, and we therefore adopt the latter
approach for simplicity.</p>
      <p>We do not include a volcanic term in the MLR model but instead choose to
exclude data from the 2-year periods following the two major tropical
volcanic eruptions during the analysis epoch: El
Chichón (data
excluded from April 1982 to March 1984) and Mt Pinatubo (data excluded from
June 1991 to May 1993). These periods are excluded from the analysis for two
reasons: firstly, some of the ozone datasets analysed implicitly exclude data
in these periods for quality control purposes, whereas others do not. For
consistency, we therefore exclude these periods for all datasets. Secondly,
removing these periods reduces the likelihood of aliasing between volcanic
and solar signals, which can be an issue within relatively short climate data
records <xref ref-type="bibr" rid="bib1.bibx6" id="paren.57"/>.</p>
      <p>We adopt the widely used F10.7 cm solar flux as a proxy for solar activity in
the MLR model. This is a more appropriate measure for variations in the UV
spectral region, the key driver of the SOR, than
other indices such as TSI <xref ref-type="bibr" rid="bib1.bibx18" id="paren.58"/>; however, it
should be noted that the F10.7 cm flux is not a direct measurement of UV
variability but rather is a proxy for variations at these wavelengths.
Throughout the manuscript the SOR is expressed as percent ozone change per
130 solar flux units (1 SFU <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>=</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn>22</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> Wm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> Hz<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) to represent
the difference between the 11-year solar cycle maximum and minimum.</p>
      <p>The 95 % confidence intervals on the SORs are estimated by
          <disp-formula id="Ch1.E2" content-type="numbered"><mml:math display="block"><mml:mrow><mml:mi>A</mml:mi><mml:mo>±</mml:mo><mml:msub><mml:mi>t</mml:mi><mml:mrow><mml:mi mathvariant="italic">α</mml:mi><mml:mo>/</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mo>,</mml:mo><mml:mi>n</mml:mi><mml:mo>-</mml:mo><mml:mo>(</mml:mo><mml:mi>k</mml:mi><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:msub><mml:msqrt><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>A</mml:mi><mml:mi>A</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:msqrt><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
        where <inline-formula><mml:math display="inline"><mml:mi>A</mml:mi></mml:math></inline-formula> is the solar regression coefficient in Eq. (<xref ref-type="disp-formula" rid="Ch1.E1"/>),
<inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>t</mml:mi><mml:mrow><mml:mi mathvariant="italic">α</mml:mi><mml:mo>/</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mo>,</mml:mo><mml:mi>n</mml:mi><mml:mo>-</mml:mo><mml:mo>(</mml:mo><mml:mi>k</mml:mi><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the critical <inline-formula><mml:math display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula> value at a confidence level,
<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>, of 0.05 with degrees of freedom <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>n</mml:mi><mml:mo>-</mml:mo><mml:mo>(</mml:mo><mml:mi>k</mml:mi><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, where <inline-formula><mml:math display="inline"><mml:mi>n</mml:mi></mml:math></inline-formula> is the number
of data points in the regression, <inline-formula><mml:math display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula> is the number of regressors, and
<inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:mi>A</mml:mi><mml:mi>A</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the variance of the estimated solar regression coefficient <inline-formula><mml:math display="inline"><mml:mi>A</mml:mi></mml:math></inline-formula>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><caption><p>Time series of the six basis functions used in the MLR model.
<bold>(a)</bold> Solar forcing based on F10.7 cm solar radio flux; <bold>(b)</bold> a
trend term based on the monthly CO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentration at Mauna Loa;
<bold>(c)</bold> equivalent effective stratospheric chlorine; <bold>(d)</bold> the
Nino 3.4 index for ENSO; <bold>(e, f)</bold> two QBO indices based on tropical
zonal winds at 50 and 30 hPa. The time series are in units of standard
deviation and the time period is 1970–2015. A volcanic term is not included
because the 2-year periods following the two major tropical volcanic eruptions in this
epoch (El Chichón and Mt Pinatubo) are excluded from the regression
analysis.</p></caption>
        <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f01.png"/>

      </fig>

      <p>As mentioned in Sect. <xref ref-type="sec" rid="Ch1.S2.SS1"/>, the SAGE II record is affected by
irregular SR and SS sampling as a function of time. This could introduce
spurious variability in the monthly mean ozone values, particularly in the
upper stratosphere, as a result of the diurnal cycle in ozone. However, many
previous regression studies of SAGE II data have not accounted for the
non-stationarity in SR/SS sampling (e.g. <xref ref-type="bibr" rid="bib1.bibx43" id="altparen.59"/>). Here, we account
for this by including an additional term in Eq. (<xref ref-type="disp-formula" rid="Ch1.E1"/>) that
quantifies the ratio between the number of SR and the total (SR <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> SS) number of
profiles used to produce each monthly mean SAGE II data point; this index can
take values between 0 and 1. An example of this index for the SAGE II v7.0
dataset at 1 hPa averaged over the tropics (30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) is
shown in Fig. <xref ref-type="fig" rid="Ch1.F2"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><caption><p>Time series of the fraction of sunrise to total
(sunrise <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> sunset) profiles used to generate monthly mean ozone values in
the tropics (30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) at 1 hPa for the SAGE II v7.0
vmr dataset.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f02.png"/>

      </fig>

      <p>One important issue for MLR analysis is the handling of possible
autocorrelation in the regression residuals and its effects on the estimation
of statistical uncertainties. A Durbin–Watson test does not reveal
significant autocorrelation in the regression residuals at most locations;
however, this is likely to be because there is a considerable fraction of
missing data points at any one location in many of the datasets analysed. In the analysis of
chemistry–climate model simulations in Part 2 of this study, for which there
is complete spatial and temporal sampling, a Durbin–Watson test
reveals significant serial correlation in the regression residuals in many
locations for lags of 1 and 2 months, particularly in the lower
stratosphere and mesosphere. This autocorrelation can lead to spurious
overestimation of the statistical significance of the regression coefficients, and we therefore include an autoregressive term in the MLR model. Given the
significant serial correlation of the residuals in the chemistry–climate
models at up to 2 months' lag in some regions, a second-order autoregressive
noise process (AR2) is used, which assumes the residuals <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> have the
following form:
          <disp-formula id="Ch1.E3" content-type="numbered"><mml:math display="block"><mml:mrow><mml:mi>r</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>=</mml:mo><mml:mi>a</mml:mi><mml:mi>r</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mi>b</mml:mi><mml:mi>r</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mi>w</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
        where <inline-formula><mml:math display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mi>b</mml:mi></mml:math></inline-formula> are constants and <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>w</mml:mi><mml:mo>(</mml:mo><mml:mi>t</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> is a white noise
process; this is the same approach employed in the recent SPARC SI<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>N
analysis of ozone trends <xref ref-type="bibr" rid="bib1.bibx53 bib1.bibx21" id="paren.60"/>. The inclusion of this term
has a very minor effect on the results for the observational datasets in Part 1 but has a greater effect for the model results in Part 2. We therefore
include it in the analysis here for consistency between both parts of the
study.</p>

      <?xmltex \floatpos{p}?><fig id="Ch1.F3" specific-use="star"><caption><p>Time series of percent tropical mean (30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N)
ozone anomalies for 1984–2004 at <bold>(a)</bold> 1 hPa (48 km),
<bold>(b)</bold> 3 hPa (40 km), <bold>(c)</bold> 5 hPa (36 km),
<bold>(d)</bold> 10 hPa (31 km), and <bold>(e)</bold> 30 hPa (24 km). Data are
shown for SAGE II v6.2 volume mixing ratios (vmr) (black), SAGE II v7.0 vmr
(red), SAGE II v6.2 number densities (nd) (blue), and SAGE II v7.0 nd
(green). The thick red lines denote the periods excluded from the MLR
analysis following major tropical volcanic eruptions. The bottom panel shows
the F10.7 cm solar flux for reference.</p></caption>
        <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f03.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><caption><p>The percent (%) annual solar-ozone response (SOR) (per 130 SFU)
for the <bold>(a, d)</bold> SAGE II v6.2 data and <bold>(b, e)</bold> SAGE II v7.0
data in terms of <bold>(a, b)</bold> number-density–altitude coordinates and
<bold>(d, e)</bold> volume-mixing-ratio–pressure coordinates. Panel <bold>(c)</bold> shows
<bold>(b)</bold> minus <bold>(a)</bold>, and panel <bold>(f)</bold> shows <bold>(e)</bold>
minus <bold>(d)</bold>. The contour interval is 1 % in panels <bold>(a, b, d, e)</bold> and 0.5 % in panels <bold>(c, f)</bold>. The hatching denotes
regions where the SOR is not statistically distinguishable from 0 at the
95 % confidence level.</p></caption>
        <?xmltex \igopts{width=355.659449pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f04.png"/>

      </fig>

</sec>
<sec id="Ch1.S4">
  <title>Results</title>
<sec id="Ch1.S4.SS1">
  <title>The SOR in SAGE II datasets</title>
      <p>Figure <xref ref-type="fig" rid="Ch1.F3"/> shows time series of monthly and tropical
(30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) mean percent ozone anomalies from 1984 to 2004
at select stratospheric levels for SAGE II v6.2 and v7.0 in units of mixing
ratios (on pressure surfaces) and number densities (on approximately
equivalent altitude surfaces). Data are only plotted where at least half of
the points within the tropical band have values in a given month. The lowest
panel shows the monthly F10.7 cm solar flux for reference.</p>
      <p><?xmltex \hack{\newpage}?>The anomalies in the two ozone number density datasets (blue and green lines)
are in close agreement in the mid-stratosphere (24, 31, and 36 km) both in
terms of high-frequency fluctuations and long-term changes. At 31 km, there
are ozone variations that are consistent with a QBO influence. At 36 and
40 km, there are variations that are visibly in phase with the solar cycle,
with relatively high ozone values from 1989 to 1992 during the solar cycle 22
maximum and lower ozone values from 1994 to 1998 during the cycle minimum.
The data show greater variance in the early and later parts of the records, and fluctuations in phase with the solar cycle are not evident from the
time series alone.</p>
      <p>The two SAGE II ozone mixing ratio datasets (black and red lines) are also in
reasonable agreement for long-term changes in the mid-stratosphere (10 and
30 hPa). However, in the upper stratosphere (1 and 3 hPa), there are
substantial differences in both short- and long-term variations. For example,
SAGE II v6.2 (black line) shows persistent negative anomalies in the early
part of the record which are not evident in v7.0 (red line). These coincide
with the 11-year solar cycle 21 minimum from 1985 to 1988. Furthermore, in
the latter part of the record, v6.2 shows relatively large-amplitude
fluctuations with mean positive anomalies from 2002 to 2004, which coincide
with the peak and subsequent declining phase of solar cycle 23. Thus, there
are differences in the evolution of ozone between the two SAGE II mixing
ratio datasets, particularly in the upper stratosphere. Overall, the two
versions of SAGE II number densities are in closer agreement than the mixing
ratio data.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><caption><p>The 95 % confidence intervals (CI) on the SORs
(SOR <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> CI) shown in Fig. <xref ref-type="fig" rid="Ch1.F4"/> for the <bold>(a, c)</bold> SAGE II v6.2 data and <bold>(b, d)</bold> SAGE II v7.0 data in terms of
<bold>(a, b)</bold> number-density–altitude coordinates and <bold>(c, d)</bold> volume-mixing-ratio–pressure coordinates. The contour interval is 0.5 %. The hatching
is as in Fig. <xref ref-type="fig" rid="Ch1.F4"/>.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f05.png"/>

        </fig>

      <p>Figure <xref ref-type="fig" rid="Ch1.F4"/>a and b show latitude–altitude plots of the annual mean SOR
for SAGE II v6.2 and v7.0 number densities, respectively. The 95 %
confidence intervals for the SORs in Fig. <xref ref-type="fig" rid="Ch1.F4"/> expressed as percent
ozone anomalies are shown in Fig. <xref ref-type="fig" rid="Ch1.F5"/>. The SORs in Fig. <xref ref-type="fig" rid="Ch1.F4"/>a
and b are generally consistent for the two datasets and show positive values
of 2–4 % across the tropical and subtropical stratosphere, except for a
region of small (<inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 1 %) negative values at 30 km in the tropics.
There is a relative maximum in the SOR of 3–4 % in the tropics at 50 km
and two off-equatorial peaks of a similar magnitude at <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 40 km and
<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>35<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>. These findings are consistent with <xref ref-type="bibr" rid="bib1.bibx45" id="text.61"/> and
<xref ref-type="bibr" rid="bib1.bibx46" id="text.62"/>, who found similar 11-year solar-like signals in tropical
upper-stratospheric ozone number densities in SAGE II v6.2 and v7.0. The
confidence intervals for the SORs in Fig. <xref ref-type="fig" rid="Ch1.F5"/>a and b show the largest
uncertainty at the equator at <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 45 km, which is close to a maximum in
the SOR. The uncertainties between 35 and 45 km are slightly larger in the
northern subtropics compared to the southern subtropics. The uncertainties in
the lower stratosphere between 22 and 28 km are smaller in magnitude, but
this is partly because the SOR is also smaller here (note the confidence
intervals are expressed as percent ozone to be directly comparable to
Fig. <xref ref-type="fig" rid="Ch1.F4"/>). Overall, the 95 % confidence intervals are around
30–50 % of the magnitude of the “best-estimate” SOR in Fig. <xref ref-type="fig" rid="Ch1.F4"/>a and b, indicating that there are
considerable uncertainties in the SOR in the SAGE II number density datasets.
This has implications for understanding the contribution of the SOR to the
atmospheric response to the solar cycle.</p>
      <p>Figure <xref ref-type="fig" rid="Ch1.F4"/>c and d show equivalent plots to
Fig. <xref ref-type="fig" rid="Ch1.F4"/>a and b for SAGE II v6.2 and v7.0 in coordinates of mixing ratios on
pressure levels. The SORs between <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 50 and 10 hPa are very similar in the
two versions and strongly resemble Fig. <xref ref-type="fig" rid="Ch1.F4"/>a and b,
with a positive SOR in the tropical lower stratosphere of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1–2 %. The
structures of the SOR between 20 and <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 7 hPa are also similar, with
subtropical maxima of 1–2 % and a distinct equatorial minimum. However, the
SORs in the upper stratosphere are markedly different between v6.2 and v7.0.
Polewards of <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>20<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> the structure of the SORs are similar in both
datasets, but the magnitude is <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 % larger in v6.2. In the tropics, the
v6.2 mixing ratio data show a large peak in the SOR in the upper stratosphere of up to
5 %, whereas the v7.0 data show a smaller SOR of 1 % in this region.</p>
      <p>The confidence intervals for the SAGE II mixing ratio SORs in Fig. <xref ref-type="fig" rid="Ch1.F5"/>c and d are generally similar to those for number
densities, with the exception of the uncertainties being considerably larger
in the tropical upper stratosphere in both datasets but particularly in SAGE II v6.2. The relatively large uncertainties in the best estimate of the SOR
would feed through to similar uncertainties in the contribution of the SOR to
the atmospheric response to the 11-year solar cycle <xref ref-type="bibr" rid="bib1.bibx17 bib1.bibx47" id="paren.63"/>. It
is therefore important to understand the causes of the differences in SOR
between the SAGE II v6.2 and v7.0 mixing ratio datasets, since this presents a limitation
for understanding and simulating the climate response to solar forcing (e.g. <xref ref-type="bibr" rid="bib1.bibx13 bib1.bibx40" id="altparen.64"/>). This is explored in the next section.</p>
<sec id="Ch1.S4.SS1.SSS1">
  <title>Differences in NMC/NCEP and MERRA-1 stratospheric temperature records</title>
      <p>Since the two versions of SAGE II show comparable SORs for
number densities, the differences between Fig. <xref ref-type="fig" rid="Ch1.F4"/>c and
d must be related to the conversion of SAGE II data to ozone
mixing ratios. As described in Sect. <xref ref-type="sec" rid="Ch1.S2"/>, SAGE II v6.2 employed
NMC/NCEP temperature data for this conversion, but this was changed to
MERRA-1 for v7.0 (see <xref ref-type="bibr" rid="bib1.bibx8" id="altparen.65"/>, for details). The differences in the
SOR in the upper stratosphere would therefore appear to be related to the use of
different temperature records in the conversion. It is known that the
evolution of stratospheric temperatures in some reanalyses show unphysical
variability and trends <xref ref-type="bibr" rid="bib1.bibx39" id="paren.66"/>, and these have been corrected for
in some solar-climate studies (e.g. <xref ref-type="bibr" rid="bib1.bibx14 bib1.bibx24" id="altparen.67"/>). However, the effect
of temperatures on the SOR in SAGE II data has not been considered
previously. Indeed, spurious variations in stratospheric temperatures in
reanalyses datasets, which are introduced through changes in the observing
system over time, could mask or enhance the SOR in SAGE II ozone mixing ratios.</p>
      <p><?xmltex \hack{\newpage}?>Figure <xref ref-type="fig" rid="Ch1.F6"/> shows time series of annual and tropical mean temperature
anomalies at select stratospheric levels (1, 2, 5, 10, 30 hPa) for the
NMC/NCEP and MERRA-1 datasets. The NMC/NCEP temperatures are those provided
with the published SAGE II data files and cover 1985–2003. MERRA-1 data were
downloaded for 1979–2013 from the NASA GFSC website. At 30 hPa, the
evolution of the two temperature records is nearly identical during the
period of overlap, with a long-term cooling trend of
<inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 0.6 K decade<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> that is strongly connected to an apparent
stepwise cooling of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 2 K between 1992 and 1994. However, at pressures
less than 30 hPa there are substantial differences between the records. The
NMC/NCEP data show exceptional behaviour between 2000 and 2003. At 1 hPa, there is
a warming of more than 3 K over this short period, which is coincident with
a warming of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 K at 2 hPa. In contrast, at 5 and 10 hPa there is a
cooling of more than 4 and 2 K, respectively, over this period. The
magnitude and vertical structure of these changes in the NMC/NCEP record
seems too inexplicable as to be related to any physical process, particularly
when compared to the variations found in the remainder of the record. Some of
these issues may be related to the method used to construct the NMC/NCEP
temperature record itself. NCEP reanalysis data were only available for
pressures greater than 10 hPa, requiring the addition of operational
analyses to extend the data to the stratopause. Data from an atmospheric
model was used to further extend the temperature data to the mesosphere, but
these levels are not considered here (see, e.g., <xref ref-type="bibr" rid="bib1.bibx8" id="altparen.68"/>, for more
details). Regardless of the
exact cause, it seems likely that some of the temperature variations in the
NMC/NCEP record are spurious, and this may impact on the diagnosed SOR in the
SAGE II v6.2 mixing ratio data.</p>
      <p>The temperature variations in MERRA-1 over the period 1985–2003 are
generally smaller in magnitude than in NMC/NCEP, with the exception of a
marked cooling at 1 hPa of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 3 K between 2001 and 2003, which is
opposite to what is seen in NMC/NCEP. This cooling in MERRA-1 leads the
decline in solar forcing during the downward phase of solar cycle 23 by
around a year and is also larger in amplitude than typical solar signals in
temperature at this level <xref ref-type="bibr" rid="bib1.bibx39" id="paren.69"/>. However, the sign is at least
consistent with the expected tendency of upper-stratospheric temperatures
during the declining phase of the solar cycle.</p>
      <p>A valid question is which representation of past stratospheric temperatures
is likely to be most realistic. <xref ref-type="bibr" rid="bib1.bibx39" id="text.70"/> compared MERRA-1 to
Stratospheric Sounding Unit (SSU) satellite data and found considerable
differences in upper-stratospheric temperature variability between the two
records. However, the NMC/NCEP data show a long-term warming trend in the
upper stratosphere, which is opposite to the cooling expected from increasing
atmospheric CO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and declining ozone abundances over this period. Both
records therefore appear to exhibit differences compared to observed
stratospheric temperature changes.</p>
      <p>The evolution of atmospheric temperatures will affect the geometric altitude
of a given pressure surface, as well as the conversion from number density to
mixing ratio. It is well known that cooling will lower the altitude of
pressure surfaces, a so-called “atmospheric shrinking” effect. Therefore, the
presence of cooling near the stratopause in MERRA-1 would tend to lead to a
greater atmospheric shrinking than for the NMC/NCEP temperatures.
Furthermore, the conversion from number density to mixing ratio is
proportional to temperature, so a positive correlation between number density
and temperature over the solar cycle would tend to increase the magnitude of
the SOR on a given pressure surface. Figure <xref ref-type="fig" rid="Ch1.F7"/> shows the annual mean
solar cycle signals in stratospheric temperatures derived for the NMC/NCEP
and MERRA-1 datasets over the period 1985–2003. Although the sign of the
temperature signals are consistent in most regions, the maximum warming in
the tropics at solar maximum occurs at 4 hPa in MERRA-1 as compared to
2 hPa in NMC/NCEP. The peak magnitude of the solar cycle temperature
response is also around 25 % smaller in MERRA-1 compared to NMC/NCEP. The
impact of these differences on the SOR in SAGE II mixing ratio data are
explored in the next section.</p>

      <?xmltex \floatpos{p}?><fig id="Ch1.F6" specific-use="star"><caption><p>Time series of tropical and annual mean temperature anomalies (K) from the
NMC/NCEP (dashed) and MERRA-1 (solid) datasets for (top to bottom) 1, 2, 5,
10, and 30 hPa. The time period is 1979–2013. The thick red lines denote
the periods excluded from the MLR analysis following major volcanic
eruptions. The bottom panel shows the F10.7 cm solar flux for reference. The
dashed vertical red lines show the period of overlap between the two datasets
from which the solar cycle signals in stratospheric temperatures in Fig. 7
are derived.</p></caption>
            <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f06.png"/>

          </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><caption><p>Eleven-year solar cycle
signals in stratospheric temperature (K) from the <bold>(a)</bold>  NMC/NCEP and
<bold>(b)</bold> MERRA-1 datasets. Shading as in Fig. <xref ref-type="fig" rid="Ch1.F4"/>. The contour
interval is 0.25 K. These temperature fields are used in the post hoc
conversion of SAGE II v6.2 number densities to mixing ratios (see
Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS2"/> for details).</p></caption>
            <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f07.png"/>

          </fig>

</sec>
<sec id="Ch1.S4.SS1.SSS2">
  <title>Dependence of SOR in SAGE II mixing ratios on temperature record</title>
      <p>To test the impact of the differences between NMC/NCEP and MERRA-1
temperatures on the SOR diagnosed in SAGE II mixing ratios, we perform our
own conversion of the SAGE II v6.2 data from number densities to mixing
ratios. Each monthly and zonal mean ozone profile is first converted to
number densities on pressure levels using the hydrostatic equation, and then
to mixing ratios on pressure levels using the ideal gas law. The MLR in
Eq. (1) is then applied to these “post hoc” converted ozone mixing ratios to derive
a SOR that can be compared to the published SAGE II mixing ratio
datasets discussed above and shown in Fig. <xref ref-type="fig" rid="Ch1.F4"/>d and e.</p>
      <p>As a first test, we convert SAGE II v6.2 number densities to mixing ratios
using the full time series of temperatures from NMC/NCEP and MERRA-1 in turn.
The SORs diagnosed from these post hoc converted datasets are shown in
Fig. <xref ref-type="fig" rid="Ch1.F8"/>a and b for NMC/NCEP and MERRA-1,
respectively, with the difference between them shown in Fig. <xref ref-type="fig" rid="Ch1.F8"/>c. These can be compared to Fig. <xref ref-type="fig" rid="Ch1.F4"/>d–f.
We stress that differences in the SORs are to be expected, since in the
published SAGE II datasets each ozone profile is converted separately before
averaging is performed, whereas here we have converted the monthly, zonally,
and latitudinally averaged ozone number density profiles.</p>
      <p>The SOR in the post hoc converted data using NMC/NCEP temperatures
(Fig. <xref ref-type="fig" rid="Ch1.F8"/>a) shows a qualitatively similar structure to
Fig. <xref ref-type="fig" rid="Ch1.F4"/>d, but the peak magnitude is underestimated by <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 2 %
in the tropical upper stratosphere. The SOR in the data converted using
MERRA-1 temperatures (Fig. <xref ref-type="fig" rid="Ch1.F8"/>b) compares more closely with the
original SAGE II v7.0 vmr dataset (Fig. <xref ref-type="fig" rid="Ch1.F4"/>e). In particular, the
reduced magnitude of the SOR in the tropical upper stratosphere is captured,
which allows us to explore how differences in the linear trends and solar
cycle signals in temperature between NMC/NCEP and MERRA-1 impact on the SOR.</p>
      <p>Figure <xref ref-type="fig" rid="Ch1.F8"/>d and e show the SOR for the SAGE II v6.2 data converted to
mixing ratios using a monthly temperature climatology from MERRA-1 added to a
latitude–height–time-dependent linear trend and solar cycle term (see
Fig. <xref ref-type="fig" rid="Ch1.F7"/>) extracted from either NMC/NCEP (Fig. <xref ref-type="fig" rid="Ch1.F8"/>d) or
MERRA-1 (Fig. <xref ref-type="fig" rid="Ch1.F8"/>e). The difference between Fig. <xref ref-type="fig" rid="Ch1.F8"/>d and e
is shown in Fig. <xref ref-type="fig" rid="Ch1.F8"/>f for reference. Figure <xref ref-type="fig" rid="Ch1.F8"/>d–f are very
similar to Fig. <xref ref-type="fig" rid="Ch1.F8"/>a–c, indicating that the majority of the
difference in SOR in Fig. <xref ref-type="fig" rid="Ch1.F8"/>c can be interpreted as being due to
differences in long-term trends and solar cycle variability in temperatures
between NMC/NCEP and MERRA-1. Further tests (not shown) show that the
diagnosed SORs are not affected by the choice of base temperature climatology
(i.e. MERRA-1 or NMC/NCEP).</p>
      <p>The remaining panels Fig. <xref ref-type="fig" rid="Ch1.F8"/>g–i and j–l show equivalent results to
Fig. <xref ref-type="fig" rid="Ch1.F8"/>d–f, but with the conversion of SAGE II v6.2 to mixing
ratios performed with the MERRA-1 temperature climatology added to either the
linear trend (Fig. <xref ref-type="fig" rid="Ch1.F8"/>g–i) or solar cycle (Fig. <xref ref-type="fig" rid="Ch1.F8"/>j–l)
components of temperature variability from the two datasets. In both of these
further tests, the SOR in the tropical upper stratosphere is larger for the
SAGE II data converted using NMC/NCEP data (Fig. <xref ref-type="fig" rid="Ch1.F8"/>g, j). This
indicates that both components of the temperature variability contribute to
the differences in SOR in Fig. <xref ref-type="fig" rid="Ch1.F8"/>c.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8" specific-use="star"><caption><p>The percent (%) annual solar-ozone response (SOR) (per 130 SFU)
in SAGE II v6.2 data converted from number densities to mixing ratios for the
period 1985–2003 using the method described in Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS2"/>. The
conversion is first conducted using full time series of monthly
<bold>(a)</bold> NMC/NCEP and <bold>(b)</bold> MERRA-1 temperatures.
Panel <bold>(c)</bold> shows <bold>(b)</bold> minus <bold>(a)</bold>. A comparison of
panels <bold>(a–c)</bold> with Fig. <xref ref-type="fig" rid="Ch1.F4"/>a–c demonstrates the performance
of the post hoc conversion. <bold>(d–f)</bold> As in panels <bold>(a–c)</bold> but
with the number density to mixing ratio conversion performed using a monthly
temperature climatology from MERRA-1 added to a linear trend and solar signal
in stratospheric temperatures extracted from <bold>(d)</bold> NMC/NCEP and
<bold>(e)</bold> MERRA-1. The remaining rows show the same as
panels <bold>(d–f)</bold> but with the conversion performed with the
<bold>(g–i)</bold> linear trend or <bold>(j–l)</bold> solar cycle temperature terms
alone. The shading is as is Fig. <xref ref-type="fig" rid="Ch1.F4"/>. The contour interval is 1 %
in the left and middle columns and 0.5 % in the right-hand column.</p></caption>
            <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f08.png"/>

          </fig>

      <p>In conclusion, the SORs in SAGE II v6.2 and v7.0 are much more consistent in
terms of number densities on altitude surfaces than they are for mixing
ratios on pressure surfaces. The differences in SORs in the latter occur
particularly in the upper stratosphere, and these have been shown to be
sensitive to the details of the temperature records used for conversion. The
long-term warming trend in the upper stratosphere in NMC/NCEP data is at odds
with the understanding of recent changes in stratospheric composition and its
impact on temperatures <xref ref-type="bibr" rid="bib1.bibx44" id="paren.71"/>; however, the peak of the solar cycle
signal in stratospheric temperatures in MERRA-1 is at a lower altitude than
predicted from theory and models. Recent analysis suggests that the
relationship between ozone and temperature in the upper stratosphere that is
anticipated from photochemical theory is more realistic for the SAGE II v7.0
mixing ratio data than for v6.2 <xref ref-type="bibr" rid="bib1.bibx12" id="paren.72"/>. Nevertheless, there remain
questions around which of the SAGE II mixing ratio datasets is likely to be
most credible for diagnosing the SOR. These results raise issues around the
representation of the SOR in the CMIP5 ozone database, which was largely
based on SAGE II v6.2 mixing ratios (<xref ref-type="bibr" rid="bib1.bibx7" id="altparen.73"/>; see also Maycock et
al., 2016).</p>

      <?xmltex \floatpos{p}?><fig id="Ch1.F9" specific-use="star"><caption><p>As in Fig. <xref ref-type="fig" rid="Ch1.F3"/> but for the three extended SAGE II number
density datasets: SAGE–GOMOS 1 (black), SAGE–GOMOS 2 (orange), and
SAGE–OSIRIS (green). The time period is 1984–2013.</p></caption>
            <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f09.png"/>

          </fig>

</sec>
</sec>
<sec id="Ch1.S4.SS2">
  <title>The SOR in extended SAGE II datasets</title>
      <p>Given the uncertainties in the SOR diagnosed for SAGE II mixing ratios
discussed above, we focus our analysis of the extended SAGE II records on the
three SI<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>N datasets that are currently available as number densities
(see Sect. <xref ref-type="sec" rid="Ch1.S2.SS1"/>): SAGE–GOMOS 1, SAGE–GOMOS 2, and
SAGE–OSIRIS. Extending SAGE II using these more recent measurements
increases the number of data points included in the MLR model by almost a
factor of 2 in the tropics and by <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 50 % in the subtropics (see
Figs. S1 and S2 in the Supplement). Figure <xref ref-type="fig" rid="Ch1.F9"/> shows time series of
monthly tropical percent ozone anomalies at select altitudes for the three
SI<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>N datasets. The datasets do not agree perfectly over the SAGE II era
(1984–2004) because the anomalies are defined relative to the entire time
series, but overall they show similar behaviour to SAGE II v7.0 number
densities (green line) in Fig. <xref ref-type="fig" rid="Ch1.F3"/>, as expected. In the post-2004
period, where either GOMOS or OSIRIS data are included, the datasets show
generally consistent behaviour in the mid-stratosphere during the overlap
period up to 2011. QBO-like variations in ozone are visible in the time
series at 24 and 31 km. At 36 km, there is a decline in ozone from 2004 to
2009 in all three datasets, with increases subsequent to this. However, in
the upper stratosphere (48 km), there are more substantial differences
between the datasets, particularly between the SAGE–GOMOS 1/2 and
SAGE–OSIRIS records. SAGE–OSIRIS shows mean positive anomalies from 2004 to
2013, particularly in the latter part of the record, whereas the two
SAGE–GOMOS datasets show negative anomalies between 2007–2010, which
coincide with the minimum of solar cycle 23. These differences in ozone
variability during the post-SAGE II period may affect the SORs diagnosed in
the extended datasets, as compared to the SAGE II v7.0 data alone
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>b).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F10" specific-use="star"><caption><p><bold>(a–c)</bold> As in Fig. <xref ref-type="fig" rid="Ch1.F4"/> but for the extended SAGE II
number density datasets: <bold>(a)</bold> SAGE–GOMOS 1,
<bold>(b)</bold> SAGE–GOMOS 2, and <bold>(c)</bold> SAGE–OSIRIS. SORs are derived
for different periods as stated in the headers. The contour interval is
1 %. <bold>(d–f)</bold> As in Fig. <xref ref-type="fig" rid="Ch1.F5"/> but for the datasets as shown
in panels <bold>(a–c)</bold>. The contour interval is 0.5 %. The hatching is
as in Fig. 4.</p></caption>
          <?xmltex \igopts{width=355.659449pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f10.png"/>

        </fig>

      <p>Figure <xref ref-type="fig" rid="Ch1.F10"/>a–c show the SORs in the three extended SAGE II datasets, and
Fig. <xref ref-type="fig" rid="Ch1.F10"/>d–f show their associated 95 % confidence intervals in
terms of percent ozone. An indication of the importance of how the satellite
records are merged for the SOR can be seen by comparing Fig. <xref ref-type="fig" rid="Ch1.F10"/>a and
b, which show SAGE–GOMOS 1 and SAGE–GOMOS 2, respectively. The SOR in
SAGE–GOMOS 1 shows a generally smoother spatial structure as compared to
SAGE–GOMOS 2, although the magnitudes are not distinguishable from one
another given the estimated confidence intervals (Fig. <xref ref-type="fig" rid="Ch1.F10"/>d–e).
Nevertheless, since statistical uncertainties in the SOR are not typically
accounted for in solar-climate studies (e.g. <xref ref-type="bibr" rid="bib1.bibx17" id="altparen.74"/>) or in climate
model ozone datasets (e.g. <xref ref-type="bibr" rid="bib1.bibx7" id="altparen.75"/>), differences in the best
estimate of the SOR between the datasets remain important to characterize.
The differences in SOR between SAGE–GOMOS 1 and 2 must arise from
differences in the data merging procedures, which are summarized by
<xref ref-type="bibr" rid="bib1.bibx53" id="text.76"/> and are described in detail by <xref ref-type="bibr" rid="bib1.bibx30" id="text.77"/> and
<xref ref-type="bibr" rid="bib1.bibx41" id="text.78"/>. Analysis of the SOR in the two SAGE–GOMOS datasets over
the SAGE II period alone (1984–2004) reveals similar differences in
magnitude and structure (not shown), which suggests that the use of SAGE II
or GOMOS as a reference to which the other record is adjusted is a key factor
for the differences in SOR in Fig. <xref ref-type="fig" rid="Ch1.F10"/>a and b. The uncertainties in
the SOR in SAGE–GOMOS 2 (Fig. <xref ref-type="fig" rid="Ch1.F10"/>e) are similar to those found in the
SAGE II v7.0 number density dataset (Fig. <xref ref-type="fig" rid="Ch1.F5"/>b), whereas the
magnitude of the uncertainties in the SOR in SAGE–GOMOS 1 (Fig. <xref ref-type="fig" rid="Ch1.F10"/>d)
are reduced compared to SAGE II v7.0, particularly in the upper stratosphere.</p>
      <p>The SOR in the SAGE–OSIRIS dataset (Fig. <xref ref-type="fig" rid="Ch1.F10"/>c) shows significant
positive values in the subtropics between <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 30 and 40 km. This is consistent
with the results of <xref ref-type="bibr" rid="bib1.bibx5" id="text.79"/> who conducted a similar MLR analysis to
assess long-term ozone trends in SAGE–OSIRIS (see also <xref ref-type="bibr" rid="bib1.bibx53" id="altparen.80"/>).
However, the SOR is smaller and less significant in the tropical upper
stratosphere and northern extratropics as compared to the two SAGE–GOMOS
datasets and the SAGE II v7.0 data. <xref ref-type="bibr" rid="bib1.bibx25" id="text.81"/> identified a significant
positive drift of 5–8 % decade<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in OSIRIS data above 35 km compared
to ozonesondes and lidar measurements, which may contribute to the
differences in SOR in the upper stratosphere.</p>
      <p>Although there are broad similarities in the SOR between the three extended
SAGE II datasets there are also important differences. This is despite the
fact that all of the datasets use SAGE II v7.0 number densities as a basis.
There is therefore a trade-off between generating the longest climate data
record possible, which is desirable for analysing quasi-decadal signals, and
the introduction of additional sources of uncertainty from combining multiple
satellite records with different sampling properties and drifts
<xref ref-type="bibr" rid="bib1.bibx21" id="paren.82"/>. There appear to be variations in ozone in the OSIRIS record
that reduce the magnitude of the SOR in the extended SAGE–OSIRIS record
compared to the SAGE II period alone. When the SAGE–GOMOS datasets are
analysed over the SAGE II period (1984–2004; not shown), SAGE–GOMOS 1 shows
the greatest resemblance to the original SAGE II v7.0 data in
Fig. <xref ref-type="fig" rid="Ch1.F4"/>b and is characterized by the smallest uncertainties of the
three datasets in the upper stratosphere, and we therefore conclude that this
record is likely the most reliable estimate of the SOR from the extended SAGE II datasets
considered.</p>
</sec>
<sec id="Ch1.S4.SS3">
  <title>The SOR in SBUV records</title>
      <p>Figure <xref ref-type="fig" rid="Ch1.F11"/> shows time series of tropical monthly percent ozone
anomalies at select stratospheric levels (as in Fig. <xref ref-type="fig" rid="Ch1.F3"/>) for the
SBUVMOD VN8.0 (black line), SBUVMOD VN8.6 (red line), and SBUV Merged
Cohesive VN8.6 (blue line) datasets. At 1 hPa, the ozone anomalies in the
different SBUV datasets are in good agreement between 1979 and 1994. After
1994, the main differences are found between the SBUVMOD VN8.0 and the two
SBUV VN8.6 datasets, the latter being largely consistent with one another. In
particular, SBUVMOD VN8.0 shows a larger positive trend in ozone from the
mid-1990s to the mid-2000s than in the SBUV VN8.6 records; this partly
coincides with the ascending phase of solar cycle 23. At 3 hPa, a comparison
of the three SBUV records reveals somewhat different behaviour. Here, the
SBUVMOD VN8.0 and SBUV Merged Cohesive VN8.6 datasets show similar ozone
variations, and instead the SBUVMOD VN8.6 is an outlier exhibiting a larger
decline in ozone compared to the other two records of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 7–8 % over
the period 1979–2012. At 5 hPa, the three SBUV datasets generally show
similar temporal variations in ozone in the early and latter parts of the
records, with some differences in offsets linked to different behaviours in
the late 1990s and early 2000s when data come from the NOAA-11, 14, 16, and
17 satellites. At 30 hPa, the three SBUV records are largely consistent with
one another in their short- and long-term variations, with some exceptions
during the 1990s when the data come mainly from the NOAA-11 and NOAA-14
satellites (see, e.g., <xref ref-type="bibr" rid="bib1.bibx53" id="altparen.83"/>).</p>

      <?xmltex \floatpos{p}?><fig id="Ch1.F11" specific-use="star"><caption><p>As in Fig. <xref ref-type="fig" rid="Ch1.F3"/> but for the SBUVMOD VN8.0 (black), SBUVMOD
VN8.6 (red), and SBUV Merged Cohesive VN8.6 (blue) datasets. The time period
is 1970–2014.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f11.png"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F12" specific-use="star"><caption><p>As in Fig. <xref ref-type="fig" rid="Ch1.F10"/> for the <bold>(a, d)</bold> SBUVMOD VN8.0,
<bold>(b, e)</bold> SBUVMOD VN8.6, and <bold>(c, f)</bold> SBUV Merged Cohesive VN8.6
datasets. SORs are derived for different periods as stated in the headers.
The contour interval in panels <bold>(a–c)</bold> is 1 % and 0.5 % in
panels <bold>(d–f)</bold>.</p></caption>
          <?xmltex \igopts{width=355.659449pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f12.png"/>

        </fig>

      <p>Figure <xref ref-type="fig" rid="Ch1.F12"/>a, b, and c show the annual mean SORs in the SBUVMOD VN8.0,
SBUVMOD VN8.6, and SBUV Merged Cohesive VN8.6 datasets, respectively.
Figure <xref ref-type="fig" rid="Ch1.F12"/>d–f show the associated 95 % confidence intervals in
terms of percent ozone. All three SBUV records show a significant positive
SOR in some parts of the upper stratosphere of up to 2–3 %. The SOR in
the tropical upper stratosphere is smaller and not highly statistically
significant in SBUVMOD VN8.6, which is in contrast to the two other records
and somewhat resembles the SOR in SAGE II v7.0 mixing ratios
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>e). The modifications to the data processing algorithm
between SBUVMOD VN8.0 and SBUVMOD VN8.6 are documented by <xref ref-type="bibr" rid="bib1.bibx3" id="text.84"/>;
these include the use of new ozone absorption cross sections, a new a priori
ozone climatology, and a new cloud-height climatology. In addition, changes
were also made to the inter-instrument calibration, which is now achieved at
the radiance level during periods of overlap between the SBUV instruments
<xref ref-type="bibr" rid="bib1.bibx10 bib1.bibx3" id="paren.85"/>. Note that the difference in SOR in the tropical upper
stratosphere between the two SBUV VN8.6 records remains when SBUVMOD VN8.6 is
analysed over the shorter 1978–2012 period (not shown), so this does not
result from the inclusion of the early BUV measurements in SBUVMOD VN8.6.</p>
      <p>The SORs in the three SBUV records show further differences between
10–50 hPa, with SBUVMOD VN8.6 showing a larger and more significant SOR,
particularly in the northern extratropics, while SBUV Merged Cohesive VN8.6
shows a weaker SOR. However, we note that the poor vertical resolution
(<inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 10 km) of the SBUV instruments at pressures greater than
<inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 15 hPa makes it challenging to resolve features in the mid and lower
stratosphere. Note that the confidence intervals for all the SBUV records are
smaller than those for SAGE II-based records (see Figs. <xref ref-type="fig" rid="Ch1.F5"/> and
<xref ref-type="fig" rid="Ch1.F10"/>d–f). This is likely to be because the number of data
points included in the MLR analysis is around 2–3 times higher for the SBUV
datasets than for the SAGE II records (see Figs. S1 and
S3 in the Supplement).</p>
      <p>It is desirable for the purposes of, e.g., chemistry–climate model evaluation
to determine which SBUV dataset might be most reliable for estimating the
annual mean SOR. <xref ref-type="bibr" rid="bib1.bibx32" id="text.86"/> analysed total column ozone measurements
from SBUVMOD VN8.0 and SBUVMOD VN8.6 and found a smaller SOR in SBUVMOD VN8.6
near-global column ozone, which appeared to be related to instrument effects
around the 1996 time frame. However, <xref ref-type="bibr" rid="bib1.bibx23" id="text.87"/> analysed the SOR in
total column ozone data and found that most of the signal is associated with
ozone changes in the lower stratosphere that are linked to dynamical
processes. Column ozone measurements are therefore unlikely to be
particularly helpful for constraining the SOR in the upper stratosphere, where
differences are found amongst many of the datasets analysed here and where
the SOR is strongly determined by photochemical processes.</p>
      <p><xref ref-type="bibr" rid="bib1.bibx53" id="text.88"/> analysed vertical profiles of long-term ozone trends in
satellite datasets and found that SBUV Merged Cohesive VN8.6 showed
negligible ozone trends at 2 hPa over 1984–1997, whereas almost all other
datasets analysed, including SBUVMOD VN8.6, showed a significant decline of
several percent per decade over this period. Instead, SBUV Merged Cohesive
VN8.6 showed larger negative ozone trends that the other datasets between
5–10 hPa. <xref ref-type="bibr" rid="bib1.bibx55" id="text.89"/> and <xref ref-type="bibr" rid="bib1.bibx53" id="text.90"/> explain how the adjustments used
to combine data from the ascending node of NOAA-11 with NOAA-9 and NOAA-14 in
SBUV Merged Cohesive VN8.6 were determined from the overlap of the descending
node of NOAA-11 with NOAA-16 because of known issues with the quality of data
from NOAA-9 and NOAA-14 <xref ref-type="bibr" rid="bib1.bibx28" id="paren.91"/>. Since the NOAA-9 and NOAA-14 data
coincide with the end of the trend analysis period used by <xref ref-type="bibr" rid="bib1.bibx53" id="text.92"/>,
this could have had a particularly pronounced impact on their linear trend
calculations but may not be as important for diagnosing the SOR.</p>
      <p>From the time series of 1 hPa ozone anomalies shown in Fig. <xref ref-type="fig" rid="Ch1.F11"/>, it
would appear that differences between the two SBUV VN8.6 datasets in the
early 2000s may be more important for determining the differences in SOR in
the tropical upper stratosphere. During this period, which coincides with the
maximum of solar cycle 22, SBUVMOD VN8.6 shows persistently more negative
ozone anomalies than SBUV Merged Cohesive VN8.6. Further analysis of the SOR
for the period up to the year 2000 (not shown) does produce a slightly larger
and more significant SOR in the tropical upper stratosphere in SBUVMOD VN8.6,
but the magnitude is still <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 % smaller than in SBUV Merged
Cohesive VN8.6, indicating that the post-2000 period alone does not explain
all differences between Fig. <xref ref-type="fig" rid="Ch1.F12"/>b and c. Based on the above factors,
it is difficult to assert which of the SBUV VN8.6 datasets is likely to be
most reliable for estimating the SOR. However, in practice the differences
between the SORs in the tropical upper stratosphere in the SBUV records are
small compared to their associated statistical uncertainties
(Fig. <xref ref-type="fig" rid="Ch1.F12"/>d–f) and small compared to the differences in SOR between
the two SAGE II mixing ratio datasets in this region. We therefore conclude
that using the longest climate data record is most favourable for diagnosing
the SOR, particularly on seasonal timescales (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS4"/>), and
we therefore adopt SBUVMOD VN8.6 for this purpose.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F13" specific-use="star"><caption><p>The percent (%) monthly solar-ozone response (SOR) (per 130 SFU)
in the SBUVMOD VN8.6 dataset for the period 1970–2012. The contour interval
is 1 %. The grey shading denotes regions where the SOR is not
statistically distinguishable from 0 at the 95 % confidence level.</p></caption>
          <?xmltex \igopts{width=355.659449pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/10021/2016/acp-16-10021-2016-f13.png"/>

        </fig>

</sec>
<sec id="Ch1.S4.SS4">
  <title>Seasonality in the solar-ozone response</title>
      <p>The analysis thus far has described the annual mean SOR in satellite ozone
datasets. However, the SOR is expected to exhibit a seasonal dependence; for
example, in regions close to photochemical steady state the annual cycle in
solar zenith angle would be expected to produce a larger SOR in the summer
hemisphere <xref ref-type="bibr" rid="bib1.bibx19" id="paren.93"/>. Furthermore, given the hypothesis that solar
variability modifies the strength of the stratospheric polar vortex
<xref ref-type="bibr" rid="bib1.bibx29" id="paren.94"/>, there may also be seasonal signatures in the SOR arising
from changes in ozone transport, particularly in the winter hemispheres.
Seasonal variations in the SOR could potentially influence the climate
response to solar forcing through coupling to radiation (e.g.
<xref ref-type="bibr" rid="bib1.bibx24" id="altparen.95"/>), and it is therefore important to characterize these in
observations and chemistry–climate models.</p>
      <p>Constraining the SOR on seasonal timescales requires high spatial and
temporal data coverage; this is to ensure that any seasonal component of the
signal can be resolved but also to increase the number of degrees of freedom
(i.e. the number of data points) available for the regression. Such coverage
is not adequately provided by limb-viewing instruments, such as SAGE II,
which have relatively sparse and infrequent sampling. The coverage is
considerably better for nadir-viewing instruments like SBUV; however, as
described above, their vertical resolution is much poorer in the middle and
lower stratosphere. There is therefore a trade-off between the information
about the SOR that can be usefully extracted from different data sources.</p>
      <p>Given the denser sampling of SBUV compared to SAGE II, we focus here on the
SBUVMOD VN8.6 dataset to examine the seasonality of the SOR.
Figure <xref ref-type="fig" rid="Ch1.F13"/> shows the monthly SOR in SBUVMOD VN8.6 for the period
1970–2012. These values are calculated by applying the MLR model to time
series for individual months, and therefore no autocorrelation term has been
included, since separate months are approximately uncorrelated from year to
year. We note that the detailed magnitudes and structure of the monthly SORs
are more sensitive to the choice of analysis epoch than for the annual mean
SOR (not shown), but the broad features generally remain consistent. The key
point to take from Fig. <xref ref-type="fig" rid="Ch1.F13"/> is that there are substantially enhanced
meridional and vertical gradients in the monthly SORs as compared to the
annual mean SOR for SBUVMOD VN8.6 in Fig. <xref ref-type="fig" rid="Ch1.F12"/>b. This is similar to the
conclusion reached by <xref ref-type="bibr" rid="bib1.bibx24" id="text.96"/>.</p>
      <p>Although much of the localized variations in the SOR are driven by dynamical
processes, it is also possible that they could feedback onto circulation
through the radiative impacts of ozone on stratospheric heating rates and
temperatures. <xref ref-type="bibr" rid="bib1.bibx24" id="text.97"/> concluded that the three chemistry–climate
models from CMIP5 that simulate strong gradients in ozone in the winter upper
stratosphere, which most closely resemble observations, tend to have
high-latitude dynamical responses to the solar cycle that are most similar to
reanalysis data. Seasonal variations in the SOR may therefore play a role in
the ability of a model to simulate the climate response to solar variability.
However, given the tight coupling between ozone and dynamics at higher
latitudes, the attribution of the importance of such radiative feedbacks is
particularly challenging. To our knowledge, the importance of this two-way
coupling for the climate response to solar variability has not been
explicitly tested. This is important to clarify because it is not known
whether it is sufficient to simply prescribe a seasonally varying SOR or
whether a fully interactive chemistry–climate model is required to
adequately capture the feedbacks between composition, radiation, and dynamics
that lead to an amplified regional response to the solar cycle. The representation of
the SOR in global climate models is discussed in more detail in Part 2 of
this study (Maycock et al., 2016).</p>
</sec>
</sec>
<sec id="Ch1.S5" sec-type="conclusions">
  <title>Conclusions</title>
      <p>The solar-ozone response (SOR) forms an important part of the climate
response to 11-year solar cycle variability through its impact on
stratospheric temperatures (e.g. <xref ref-type="bibr" rid="bib1.bibx47 bib1.bibx17" id="altparen.98"/>). This papers forms
the first of a two-part study that aims to quantify the SOR in current
satellite observations and chemistry–climate models. Part 1 has focused on
comparing the SOR in recently updated and/or extended versions of long-term
satellite ozone datasets (e.g. SAGE II, SBUV) with their previous
counterparts (e.g. <xref ref-type="bibr" rid="bib1.bibx49 bib1.bibx1" id="altparen.99"/>).</p>
      <p>The SAGE II dataset has been widely used for ozone studies because of its
long-term stability. SAGE II ozone data are available as number densities on
altitude levels and post-processed to mixing ratios on pressure levels. The
SAGE II version 6.2 (v6.2) mixing ratio dataset shows a positive annual mean
SOR with a peak magnitude of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 5 % near the tropical stratopause.
However, the more recent SAGE II v7.0 dataset shows a substantially smaller
SOR at the tropical stratopause of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 %. Conversely, the SORs in the
equivalent SAGE II number density datasets are much more consistent for v6.2
and v7.0 and show a three-peaked structure in the tropics and subtropics with a
magnitude of up to 3–4 %.</p>
      <p>By applying a post hoc method to convert SAGE II number densities to mixing
ratios, we have shown that the differences in SOR are strongly determined by
the change in independent temperature record used to convert SAGE II number
densities to mixing ratios: v6.2 uses NMC/NCEP and v7.0 uses MERRA-1
temperatures. Differences between these temperature records in both long-term
trends and solar cycle variations contribute to the changes in SOR described
above. Since both temperature records contain known issues (e.g.
<xref ref-type="bibr" rid="bib1.bibx8 bib1.bibx39" id="altparen.100"/>), we conclude that the latest SAGE II v7.0 ozone
number densities are likely to be most reliable for estimating the SOR at the
present time. This is an important conclusion because several of the existing
ozone datasets developed for use in global climate models have been based on
SAGE II v6.2 mixing ratio data, including the dataset developed for CMIP5
simulations <xref ref-type="bibr" rid="bib1.bibx7" id="paren.101"/>.</p>
      <p>We further analysed the annual mean SOR in three extended SAGE II datasets
that have merged more recent GOMOS (2002–2011) or OSIRIS (2002–2013) data
with SAGE II v7.0 number densities. Two SAGE–GOMOS datasets were analysed
that adopt different methods for merging the satellite records
<xref ref-type="bibr" rid="bib1.bibx30 bib1.bibx41" id="paren.102"/>. These records show broadly similar SORs, but the
dataset that uses SAGE II as a reference and adjusts GOMOS using seasonally
varying offsets at each latitude and altitude <xref ref-type="bibr" rid="bib1.bibx41" id="paren.103"/> was found to
have a SOR with a noisier spatial structure. The SAGE–OSIRIS dataset
<xref ref-type="bibr" rid="bib1.bibx5" id="paren.104"/> shows a significant positive SOR of <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 2 % between
30 and 40 km but a weaker and less significant SOR in the tropical upper
stratosphere than is found in the SAGE–GOMOS datasets. Thus, the inclusion
of OSIRIS data results in a markedly different SOR to that found in the
SAGE II v7.0 number densities that underpin the first part of the record.
Given these various issues, we conclude that the SAGE–GOMOS 1 dataset
<xref ref-type="bibr" rid="bib1.bibx30" id="paren.105"/> is likely to be the most reliable extended SAGE II dataset for
estimating the SOR at the present time.</p>
      <p>Analysis of the recently released SBUVMOD VN8.6 data produced by NASA show a
SOR in the tropical upper stratosphere that is smaller by <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 %
compared to the previous SBUVMOD VN8.0 data <xref ref-type="bibr" rid="bib1.bibx49" id="paren.106"/>. However, the
SBUV Merged Cohesive VN8.6 dataset from NOAA, which takes a different
approach for combining the individual SBUV VN8.6 records, shows a SOR that
more closely matches SBUVMOD VN8.0. Nevertheless, the differences in the
magnitude of the SOR between the various SBUV records are generally smaller
than those between the SAGE II v6.2 and v7.0 mixing ratio datasets and are
not highly statistically significant given the estimated uncertainties in the
SOR derived from the regression model. We therefore suggest that the SBUVMOD
VN8.6 dataset is most appropriate for analysing the SOR since it is the
longest of the currently available SBUV VN8.6 records (1970–2012).</p>
      <p>Analysis of the SOR on monthly timescales in the SBUVMOD VN8.6 dataset
reveals substantially larger horizontal and vertical gradients in the SOR,
particularly in the winter extratropics. <xref ref-type="bibr" rid="bib1.bibx24" id="text.107"/> analysed CMIP5 models
with interactive chemistry and concluded that the models with seasonal
variations in the SOR that best matched observations simulated changes in
high-latitude zonal winds over the solar cycle that more closely resemble
reanalysis data. Seasonal variations in the SOR may therefore be important
for the climate response to solar variability, but the quantitative
importance of this feedback for stratospheric dynamics remains to be tested.</p>
      <p>To allow for a realistic representation of the climate impacts of solar
variability in models, simulations should include the effects of both the SOR
and variations in spectral solar irradiance <xref ref-type="bibr" rid="bib1.bibx35" id="paren.108"/>. Our results raise
issues for how to best represent the SOR in “non-interactive” climate
models for which the SOR much be externally prescribed. For example, ozone
databases for climate models are usually created using a variety of ozone
measurements, and therefore implicitly include a representation of the SOR
that emerges from whichever combinations of data are included (e.g.
<xref ref-type="bibr" rid="bib1.bibx7 bib1.bibx4" id="altparen.109"/>). However, the differences in the magnitude and
structure of the SOR between various satellite datasets as described here
would likely result in different climate responses to solar forcing. There is
therefore a need for new studies to explore the effects of uncertainties in
the SOR for climate simulation, particularly in light of the substantial, but
largely unexplained, spread in climate responses to the 11-year solar cycle
across CMIP5 models <xref ref-type="bibr" rid="bib1.bibx40 bib1.bibx24" id="paren.110"/>.</p>
</sec>
<sec id="Ch1.S6">
  <title>Data availability</title>
      <p>The SAGE II and SBUVMOD datasets used in this study are all publicly
available online. Citations or links to data sources have been included
wherever possible. The SI<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>N ozone datasets
were kindly provided by Fiona Tummon. Users wishing to access the SI<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>N
datasets should contact the Principal Investigators
directly.</p>
</sec>

      
      </body>
    <back><app-group>
        <supplementary-material position="anchor"><p><bold>The Supplement related to this article is available online at <inline-supplementary-material xlink:href="http://dx.doi.org/10.5194/acp-16-10021-2016-supplement" xlink:title="pdf">doi:10.5194/acp-16-10021-2016-supplement</inline-supplementary-material>.</bold></p></supplementary-material>
        </app-group><ack><title>Acknowledgements</title><p>Amanda C. Maycock acknowledges funding from an AXA Postdoctoral Fellowship,
the ERC ACCI Grant Project No. 267760, and a NERC Independent Research
Fellowship (NE/M018199/1). Amanda C. Maycock also acknowledges funding from
the COST action ES1005 “Towards a more complete assessment of the impact of
solar variability on the Earth's climate” (TOSCA) for a Short-term
Scientific Mission to GEOMAR in September 2014 which initiated this work.
Parts of the work at GEOMAR Helmholtz Centre for Ocean Research Kiel was
performed within the Helmholtz University Young Investigators Group NATHAN,
funded by the Helmholtz Association and GEOMAR. We thank Fiona Tummon for
kindly providing the merged ozone datasets that formed part of the
SI<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>N initiative. We thank Stacey Frith for
providing useful information about the SBUV records. We also thank the many
instrument scientists and groups who have contributed to the development of
long-term satellite ozone datasets and who have kindly made their data
available for this study. The authors thank J. Zawodny, J. Lean, and the two
anonymous reviewers for their detailed review comments, which improved the
manuscript.
<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?> Edited by: M. Dameris
<?xmltex \hack{\newline}?> Reviewed by: J. Zawodny, J. Lean, and two anonymous
referees</p></ack><ref-list>
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    <!--<article-title-html>The representation of solar cycle signals in stratospheric ozone – Part 1: A comparison of recently updated satellite observations</article-title-html>
<abstract-html><p class="p">Changes in
incoming solar ultraviolet radiation over the 11-year solar cycle affect
stratospheric ozone abundances. It is important to quantify the magnitude,
structure, and seasonality of the associated solar-ozone response (SOR) to
understand the impact of the 11-year solar cycle on climate. Part 1 of this
two-part study uses multiple linear regression analysis to extract the SOR in
a number of recently updated satellite ozone datasets covering different
periods within the epoch 1970 to 2013. The annual mean SOR in the updated
version 7.0 (v7.0) Stratospheric Aerosol and Gas Experiment (SAGE) II number
density dataset (1984–2004) is very consistent with that found in the
previous v6.2. In contrast, we find a substantial decrease in the magnitude
of the SOR in the tropical upper stratosphere in the SAGE II v7.0 mixing
ratio dataset ( ∼  1 %) compared to the v6.2 ( ∼  4 %). This
difference is shown to be largely attributable to the change in the
independent stratospheric temperature dataset used to convert SAGE II ozone
number densities to mixing ratios. Since these temperature records contain
substantial uncertainties, we suggest that datasets based on SAGE II number
densities are currently most reliable for evaluating the SOR. We further
analyse three extended ozone datasets that combine SAGE II v7.0 number
densities with more recent GOMOS (Global Ozone Monitoring by Occultation of
Stars) or OSIRIS (Optical Spectrograph and Infrared Imager System)
measurements. The extended SAGE–OSIRIS dataset (1984–2013) shows a smaller
and less statistically significant SOR across much of the tropical upper
stratosphere compared to the SAGE II data alone. In contrast, the two
SAGE–GOMOS datasets (1984–2011) show SORs that are in closer agreement with
the original SAGE II data and therefore appear to provide a more reliable
estimate of the SOR. We also analyse the SOR in the recent Solar Backscatter
Ultraviolet Instrument (SBUV) Merged Ozone Dataset (SBUVMOD) version 8.6
(VN8.6) (1970–2012) and SBUV Merged Cohesive VN8.6 (1978–2012) datasets and
compare them to the previous SBUVMOD VN8.0 (1970–2009). Over their full
lengths, the three records generally agree in terms of the broad magnitude
and structure of the annual mean SOR. The main difference is that SBUVMOD
VN8.6 shows a smaller and less significant SOR in the tropical upper
stratosphere and therefore more closely resembles the SAGE II v7.0 mixing
ratio data than does the SBUV Merged Cohesive VN8.6, which has a more
continuous SOR of  ∼  2 % in this region. The sparse spatial and
temporal sampling of limb satellite instruments prohibits the extraction of
sub-annual variations in the SOR from SAGE-based datasets. However, the
SBUVMOD VN8.6 dataset suggests substantial month-to-month variations in the
SOR, particularly in the winter extratropics, which may be important for the
proposed high-latitude dynamical response to the solar cycle. Overall, the
results highlight substantial uncertainties in the magnitude and structure of
the observed SOR from different satellite records. The implications of these
uncertainties for understanding and modelling the effects of solar
variability on climate should be explored.</p></abstract-html>
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