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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" xml:lang="en" dtd-version="3.0" article-type="research-article"><?xmltex \bartext{Research article}?>
  <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-23-5101-2023</article-id><title-group><article-title>The response of the North Pacific jet and stratosphere-to-troposphere
transport of ozone over western North America to RCP8.5 climate forcing</article-title><alt-title>The response of the North Pacific jet and stratosphere-to-troposphere
transport</alt-title>
      </title-group><?xmltex \runningtitle{The response of the North Pacific jet and stratosphere-to-troposphere
transport}?><?xmltex \runningauthor{D.~Elsbury et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1 aff2">
          <name><surname>Elsbury</surname><given-names>Dillon</given-names></name>
          <email>dillon.elsbury@noaa.gov</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Butler</surname><given-names>Amy H.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-3632-0925</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff3">
          <name><surname>Albers</surname><given-names>John R.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-8383-3379</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff3">
          <name><surname>Breeden</surname><given-names>Melissa L.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Langford</surname><given-names>Andrew O'Neil</given-names></name>
          
        </contrib>
        <aff id="aff1"><label>1</label><institution>Cooperative Institute for Research in Environmental Sciences (CIRES), <?xmltex \hack{\break}?> University of Colorado Boulder, Boulder, Colorado 80309, USA</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>NOAA Chemical Sciences Laboratory (CSL), Boulder, Colorado 80305, USA</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>NOAA Physical Sciences Laboratory (PSL), Boulder, Colorado 80305, USA</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Dillon Elsbury (dillon.elsbury@noaa.gov)</corresp></author-notes><pub-date><day>4</day><month>May</month><year>2023</year></pub-date>
      
      <volume>23</volume>
      <issue>9</issue>
      <fpage>5101</fpage><lpage>5117</lpage>
      <history>
        <date date-type="received"><day>30</day><month>September</month><year>2022</year></date>
           <date date-type="rev-request"><day>22</day><month>November</month><year>2022</year></date>
           <date date-type="rev-recd"><day>23</day><month>February</month><year>2023</year></date>
           <date date-type="accepted"><day>27</day><month>March</month><year>2023</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2023 </copyright-statement>
        <copyright-year>2023</copyright-year>
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://acp.copernicus.org/articles/.html">This article is available from https://acp.copernicus.org/articles/.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d1e134">Stratosphere-to-troposphere transport (STT) is an important source
of ozone for the troposphere, particularly over western North America. STT
in this region is predominantly controlled by a combination of the
variability and location of the Pacific jet stream and the amount of ozone
in the lower stratosphere, two factors which are likely to change if
greenhouse gas concentrations continue to increase. Here we use Whole
Atmosphere Community Climate Model experiments with a tracer of
stratospheric ozone (O3S) to study how end-of-the-century Representative
Concentration Pathway (RCP) 8.5 sea surface temperatures (SSTs) and
greenhouse gases (GHGs), in isolation and in combination, influence STT of
ozone over western North America relative to a preindustrial control
background state.</p>

      <p id="d1e137">We find that O3S increases by up to 37 % during late winter at 700 hPa
over western North America in response to RCP8.5 forcing, with the increases
tapering off somewhat during spring and summer. When this response to RCP8.5
greenhouse gas forcing is decomposed into the contributions made by future
SSTs alone versus future GHGs alone, the latter are found to be primarily
responsible for these O3S changes. Both the future SSTs alone and the future
GHGs alone accelerate the Brewer–Dobson circulation, which modifies
extratropical lower-stratospheric ozone mixing ratios. While the future GHGs
alone promote a more zonally symmetric lower-stratospheric ozone change due
to enhanced ozone production and some transport, the future SSTs alone
increase lower-stratospheric ozone predominantly over the North Pacific via
transport associated with a stationary planetary-scale wave. Ozone
accumulates in the trough of this anomalous wave and is reduced over the
wave's ridges, illustrating that the composition of the lower-stratospheric
ozone reservoir in the future is dependent on the phase and position of the
stationary planetary-scale wave response to future SSTs alone, in addition
to the poleward mass transport provided by the accelerated Brewer–Dobson
circulation. Further, the future SSTs alone account for most changes to the
large-scale circulation in the troposphere and stratosphere compared to the
effect of future GHGs alone. These changes include modifying the position
and speed of the future North Pacific jet, lifting the tropopause,
accelerating both the Brewer–Dobson circulation's shallow and deep branches,
and enhancing two-way isentropic mixing in the stratosphere.</p>
  </abstract>
    
<funding-group>
<award-group id="gs1">
<funding-source>National Science Foundation</funding-source>
<award-id>1756958</award-id>
</award-group>
<award-group id="gs2">
<funding-source>National Oceanic and Atmospheric Administration</funding-source>
<award-id>NA17OAR4320101</award-id>
<award-id>NA22OAR4320151</award-id>
</award-group>
</funding-group>
</article-meta>
  </front>
<body>
      

<?pagebreak page5102?><sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e149">Tropospheric ozone is a pollutant harmful to humans and vegetation;
therefore, understanding its response to climate change has important
implications for future air quality (Fleming et al., 2018; Zanis et al., 2022). Future tropospheric ozone amounts are affected by multiple processes,
including anthropogenic emissions and changes to the large-scale
circulation, which in turn are dependent on the choice of model and climate
change scenario (Young et al., 2018). For high-end emissions scenarios
(Representative Concentration Pathway (RCP) 8.5), recent chemistry–climate
models project an increase in Northern Hemisphere tropospheric ozone
(Archibald et al., 2020), largely due to enhanced methane emissions
(Winterstein et al., 2019) but also due to stronger transport of
stratospheric ozone into the troposphere (Griffiths et al., 2021).</p>
      <p id="d1e152">Enhanced stratosphere-to-troposphere transport (STT) of ozone is expected in
the future, due in part to more frequent tropopause folding (Akritidis et al., 2019) but also due to higher ozone mixing ratios in the lower
stratosphere. Since the amount of ozone in the lower extratropical
stratospheric “reservoir”, often measured on the 350 K isentrope, is
positively correlated with the amount of ozone contained in intrusions of
stratospheric air exchanged into the troposphere (Albers et al., 2018),
larger lower-stratospheric ozone mixing ratios should coincide with more STT
of ozone. A diverse set of physical and chemical processes is anticipated to
have the net effect of increasing future lower-stratospheric ozone mixing
ratios in the extratropics; these processes include enhanced downwelling
associated with the acceleration of the Brewer–Dobson circulation (BDC) (Abalos et al., 2020), two-way isentropic mixing (Eichinger et al., 2019; Ball et al., 2020; Dietmüller et al., 2021), enhanced ozone production associated with
stratospheric cooling (Rind et al., 1990; Jonsson et al., 2004; Oman et al., 2010), chemical impacts of increasing methane and nitrous oxide
concentrations (Revell et al., 2012; Butler et al., 2016; Winterstein et al., 2019), and expected emissions reductions of ozone-depleting substances
(ODSs) (Banerjee et al., 2016; Meul et al., 2018; Fang et al., 2019; Griffiths
et al., 2020; Dietmüller et al., 2021).</p>
      <p id="d1e155">While the mechanisms influencing future lower-stratospheric ozone changes
are fairly well established in a zonally averaged sense, it is less evident
what role regional dynamical and chemical zonal asymmetries will play in
future STT. Historically, one of the key regions where stratospheric mass
fluxes enter the lower free troposphere is over western North America
(Sprenger and Wernli 2003; Lefohn et al., 2011; Škerlak et al., 2014).
Tropopause folding and STT maximize over this region during spring, when the
North Pacific jet transitions from a strong and latitudinally narrow band of
westerlies to a weaker and latitudinally broad jet (Newman and Sardeshmukh,
1998; Breeden et al., 2021). Intrusions here have been observed to enhance
free tropospheric ozone concentrations beyond 30 ppb (Knowland
et al., 2017; Langford et al., 2017; Zhang et al., 2020; Xiong et al., 2022;
Langford et al., 2022). When combined with background ozone concentrations,
which are also affected by regional precursor emissions, vegetation, and
upwind transport (Cooper et al., 2010; Langford et al., 2017), ozone
concentrations may exceed the surface 8 h National Ambient Air
Quality Standard (EPA, 2006).</p>
      <p id="d1e158">It is established that the subtropical and eddy-driven jets' response to
climate change will vary by region and season (Akritidis et al., 2019; Harvey
et al., 2020). However, it is not yet known how regional jet changes, such as
the spring transition of the North Pacific jet, combined with changes to the
lower-stratospheric ozone reservoir may affect STT regionally in the
future. In this study, we use a set of National Center for Atmospheric
Research (NCAR) Whole Atmosphere Community Climate Model (WACCM) experiments
described in Sect. 2, which include fully interactive chemistry and a
tracer of stratospheric ozone (O3S), to evaluate how RCP8.5 sea surface
temperatures (SSTs) alone and RCP8.5 greenhouse gases (GHGs) alone, and also
in combination, influence STT of ozone over western North America. Strictly
speaking, warming SSTs in high-emission scenarios such as RCP8.5 result from
the increased GHG emissions. However, when considered independently of each
other (by holding one fixed while changing the other), the SSTs alone and
the GHGs alone have distinct impacts on the future atmosphere, with the SSTs
alone being disproportionately responsible for future subtropical jet
changes and amplification of the BDC's shallow branch (Oberländer et al., 2013; Chrysanthou et al., 2020) and the GHGs alone being primarily
responsible for production of stratospheric ozone and amplification of the
BDC's deep branch (Winterstein et al., 2019; Abalos et al., 2021;
Dietmüller et al., 2021). Therefore, as is shown in Sect. 3, each
forcing, either dynamically or chemically, influences processes that affect
STT over western North America. Section 4 synthesizes the results, namely
that the RCP8.5 GHGs alone are primarily responsible for future increases in
lower-tropospheric O3S over western North America despite the RCP8.5 SSTs
alone disproportionately accounting for future dynamical changes in the
troposphere and stratosphere, including those associated with the North
Pacific jet's spring transition.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Methods</title>
      <p id="d1e169">We compare output from three different 60-year integrations using NCAR WACCM
(Table 1). The version of WACCM used in this study uses a horizontal
resolution of 1.9<inline-formula><mml:math id="M1" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> latitude by 2.5<inline-formula><mml:math id="M2" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> longitude with 70
vertical layers and a model top near 140 km (Mills et al., 2017; Richter et al., 2017). These experiments do not include an internally generated or
prescribed quasi-biennial oscillation; the climatological tropical
stratospheric winds are weakly easterly. WACCM has fully<?pagebreak page5103?> interactive
chemistry in the middle atmosphere using the Model for Ozone And Related
chemical Tracers (MOZART3) and a limited representation of tropospheric
chemistry (Kinnison et al., 2007). The chemistry module in WACCM includes a
stratospheric ozone tracer (O3S), which is used to quantify STT of ozone.
O3S is set equal to the fully interactive stratospheric ozone at each model
time step. Once it crosses the tropopause, O3S decays at the tropospheric
chemistry rate and is lost due to dry deposition. O3S represents an upper
bound on the contribution of the stratosphere to tropospheric ozone, in
large part because it is missing some tropospheric chemistry that would
likely reduce its lifetime.</p>
      <p id="d1e190">To isolate the signal of atmospheric tracers to external forcings above the
“noise” of internal atmospheric variability, we have run “time-slice”
simulations forced by fixed SSTs, allowing us to both generate longer
simulations than more computationally expensive coupled atmosphere–ocean
simulations and remove year-to-year fluctuations in ocean sea surface
temperatures that may arise internally. Each time-slice simulation has been
run for 60 years, with 10 years of spin-up (which is sufficient for
initialized atmosphere-only runs).</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><?xmltex \currentcnt{1}?><label>Table 1</label><caption><p id="d1e196">Each experiment is prescribed with fixed repeating annual cycles of
the time-averaged SST from the years listed in column three. Greenhouse gas
mixing ratios coinciding with the years indicated in column four are shown
for four of the species in columns five through eight.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="8">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="right"/>
     <oasis:colspec colnum="8" colname="col8" align="right"/>
     <oasis:thead>
       <oasis:row>
         <oasis:entry colname="col1">Name</oasis:entry>
         <oasis:entry colname="col2">Experiment</oasis:entry>
         <oasis:entry colname="col3">SST</oasis:entry>
         <oasis:entry colname="col4">GHG</oasis:entry>
         <oasis:entry colname="col5">Methane</oasis:entry>
         <oasis:entry colname="col6">Nitrous</oasis:entry>
         <oasis:entry colname="col7">Carbon</oasis:entry>
         <oasis:entry colname="col8">Cl<inline-formula><mml:math id="M3" display="inline"><mml:msub><mml:mi/><mml:mi>y</mml:mi></mml:msub></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">type</oasis:entry>
         <oasis:entry colname="col3">years</oasis:entry>
         <oasis:entry colname="col4">year</oasis:entry>
         <oasis:entry colname="col5">(ppb)</oasis:entry>
         <oasis:entry colname="col6">oxide</oasis:entry>
         <oasis:entry colname="col7">dioxide</oasis:entry>
         <oasis:entry colname="col8">(ppb)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6">(ppb)</oasis:entry>
         <oasis:entry colname="col7">(ppm)</oasis:entry>
         <oasis:entry colname="col8"/>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">EXP1</oasis:entry>
         <oasis:entry colname="col2">Preindustrial</oasis:entry>
         <oasis:entry colname="col3">1840–1870</oasis:entry>
         <oasis:entry colname="col4">1850</oasis:entry>
         <oasis:entry colname="col5">790</oasis:entry>
         <oasis:entry colname="col6">275</oasis:entry>
         <oasis:entry colname="col7">285</oasis:entry>
         <oasis:entry colname="col8">0.46</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">EXP2</oasis:entry>
         <oasis:entry colname="col2">RCP8.5</oasis:entry>
         <oasis:entry colname="col3">2070–2090</oasis:entry>
         <oasis:entry colname="col4">2090</oasis:entry>
         <oasis:entry colname="col5">3632</oasis:entry>
         <oasis:entry colname="col6">421</oasis:entry>
         <oasis:entry colname="col7">844</oasis:entry>
         <oasis:entry colname="col8">1.36</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">EXP3</oasis:entry>
         <oasis:entry colname="col2">RCP8.5 SSTs</oasis:entry>
         <oasis:entry colname="col3">2070–2090</oasis:entry>
         <oasis:entry colname="col4">1850</oasis:entry>
         <oasis:entry colname="col5">790</oasis:entry>
         <oasis:entry colname="col6">275</oasis:entry>
         <oasis:entry colname="col7">285</oasis:entry>
         <oasis:entry colname="col8">0.46</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><?xmltex \gdef\@currentlabel{1}?></table-wrap>

      <p id="d1e397">The first experiment (EXP1) is a preindustrial control simulation forced
with the year 1850 GHGs and a fixed repeating annual cycle of SSTs and sea ice
created from the time-averaged 1840–1870 period. The second experiment
(EXP2) is forced with a fixed repeating annual cycle of SSTs and sea ice based
on the time-averaged 2070–2090 period from a fully coupled run of the
same version of WACCM and GHG concentrations at the year 2090 from the RCP8.5
scenario. The RCP8.5 scenario represents a “worst-case” future scenario in
which the radiative forcing imbalance between year 2100 and 1850 is 8.5 W m<inline-formula><mml:math id="M4" 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> due to marked increases in concentrations of carbon dioxide,
nitrous oxide, and methane by the end of the century (van Vuuren et al., 2011). We chose this extreme scenario in order to simulate the “upper
bounds” of the response. There are also increased concentrations of
ozone-depleting substances (ODSs; e.g., chlorofluorocarbons) relative to the
preindustrial experiment, due to the long lifetimes of these substances,
which were emitted prior to the Montreal Protocol. Non-methane ozone
precursor emissions, the solar flux, and stratospheric aerosol
concentrations are held fixed to levels of the year 1850. The difference between
EXP2 and EXP1 includes the atmospheric response to higher GHGs, more ODSs,
and warmer SSTs.</p>
      <p id="d1e412">One additional experiment is used to disentangle the atmospheric response to
future GHGs (which includes ODSs) alone from future SSTs alone. This
experiment (EXP3) is identical to the RCP8.5 experiment (EXP2), except that
GHGs are held fixed to concentrations in the year 1850. By comparing EXP3 to EXP1,
we can isolate the atmospheric response to the future SST increase only.
This response to SSTs alone, which strictly speaking results from having
higher GHG concentrations, constitutes one component of the response to full
RCP8.5 forcing. By comparing the experiment in which the RCP8.5 SSTs are the
only forcing (EXP3) to the full RCP8.5 experiment (EXP2), the response to
GHGs (and ODSs) alone is approximated; the 4.6 times, 1.5 times, 3 times, and 3 times increases
relative to the preindustrial conditions in CH<inline-formula><mml:math id="M5" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:math></inline-formula>, N<inline-formula><mml:math id="M6" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>O, CO<inline-formula><mml:math id="M7" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>,
and Cl<inline-formula><mml:math id="M8" display="inline"><mml:msub><mml:mi/><mml:mi>y</mml:mi></mml:msub></mml:math></inline-formula>, respectively, are the only differences between these
experiments (Table 1). Herein, the ODSs are binned as part of the “GHG
alone”. Therefore, the ozone response to GHGs alone is a bulk ozone
response to the chemical and radiative effects of CH<inline-formula><mml:math id="M9" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:math></inline-formula>, N<inline-formula><mml:math id="M10" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>O,
CO<inline-formula><mml:math id="M11" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, and Cl<inline-formula><mml:math id="M12" display="inline"><mml:msub><mml:mi/><mml:mi>y</mml:mi></mml:msub></mml:math></inline-formula>, each of which have interfering effects on
ozone. Broadly speaking, enhanced methane increases ozone below 40 km through multiple pathways (Portmann and Solomon, 2007; Fleming et al., 2011; Revell et al., 2012; Winterstein et al., 2019), increased N<inline-formula><mml:math id="M13" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>O
and Cl<inline-formula><mml:math id="M14" display="inline"><mml:msub><mml:mi/><mml:mi>y</mml:mi></mml:msub></mml:math></inline-formula> enhance stratospheric ozone loss (Butler et al., 2016;
Morgenstern et al., 2018), and more CO<inline-formula><mml:math id="M15" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> increases ozone by cooling the
stratosphere, thereby reducing ozone loss (Jonsson et al., 2004).</p>
      <p id="d1e515">Note that we derive our response to GHGs alone as the residual between EXP3,
which includes RCP8.5 SSTs only, and EXP2, which includes full RCP8.5
forcing. If the SST forcing and GHG forcings interact non-linearly, the
response to GHGs alone as we define it (EXP2–EXP3) may be different from
the response to GHGs alone that could be obtained by comparing a
preindustrial experiment to an experiment with RCP8.5 greenhouse gases and
SSTs fixed to 1850 conditions. The additivity of the response to SSTs alone
and the response to GHGs alone will have to be assessed in future work.</p>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Decomposing the jet into late-winter, spring, and summer phases</title>
      <p id="d1e525">Breeden et al. (2021) showed that the mass of stratospheric air entering the
lower troposphere over western North America is 3 times larger during
the jet's spring transition phase as opposed to its late-winter or summer
phases. This peak in mass transport is associated with enhanced synoptic-scale wave activity in the upper troposphere, tropopause folds that reach
deeper into the troposphere, and a deeper planetary boundary layer. Because
the seasonal evolution of the North Pacific jet impacts STT over western
North America, in all of our analyses we consider changes in all fields as
a function of the three phases of the seasonal transition of the North
Pacific jet, as they are defined in Breeden et al. (2021). Therefore, the
differences in transport arising from timing of the jet transition are
inherently taken into account.</p>
      <p id="d1e528">Figure 1 shows the seasonal evolution of the North Pacific jet in the
preindustrial control (EXP1) and in the RCP8.5 experiment (EXP2). The jet is
separated into winter, spring, and summer phases using the principal
component time series associated with the first empirical orthogonal
function (EOF) of the daily 200 hPa zonal winds averaged over the North
Pacific region (100–280<inline-formula><mml:math id="M16" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E and 10–70<inline-formula><mml:math id="M17" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N). The zonal wind anomalies used for the EOF analysis are
calculated with respect to the February to June years 11–60 average,<?pagebreak page5104?> rather
than a daily climatology, in order to deliberately preserve the seasonal
cycle that emerges as the first EOF. The associated principal component time
series (PC1), calculated by projecting the gridded zonal wind for either the
preindustrial control (EXP1) (Fig. 1d) or the RCP8.5 experiment (EXP2) (Fig. 1e) at each time step onto each experiment's EOF1, are smoothed with a
5 d running mean.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><?xmltex \currentcnt{1}?><?xmltex \def\figurename{Figure}?><label>Figure 1</label><caption><p id="d1e551">Spring transition of the North Pacific jet in the preindustrial
control (EXP1) and the RCP 8.5 experiment (EXP2). Panels <bold>(a)</bold>–<bold>(c)</bold> show preindustrial
200 hPa zonal winds subsampled for the jet's winter phase (PC1 <inline-formula><mml:math id="M18" display="inline"><mml:mi mathvariant="italic">&gt;</mml:mi></mml:math></inline-formula> 1<inline-formula><mml:math id="M19" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>), spring phase (PC1 <inline-formula><mml:math id="M20" display="inline"><mml:mi mathvariant="italic">&lt;</mml:mi></mml:math></inline-formula> 0.5<inline-formula><mml:math id="M21" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M22" display="inline"><mml:mi mathvariant="italic">&gt;</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M23" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.5<inline-formula><mml:math id="M24" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>), and summer phase (PC1 <inline-formula><mml:math id="M25" display="inline"><mml:mi mathvariant="italic">&lt;</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M26" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1<inline-formula><mml:math id="M27" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>). Panel <bold>(d)</bold> shows the
temporal evolution of PC1 in the preindustrial control (EXP1), with the mean
PC1 shown in black, PC1 for each year shown in blue, and the 2.5 % and
97.5 % confidence intervals calculated by bootstrapping with replacement
(10 000 times for each day) shown in gray. The average difference between
the 2.5 % and 97.5 % confidence intervals for each <inline-formula><mml:math id="M28" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 2-week period (referred to as “spread”) are shown above panel <bold>(d)</bold>. Panel <bold>(e)</bold>
is the same as panel <bold>(d)</bold> but for the RCP8.5 experiment (EXP2). In addition,
the percent change between the RCP8.5 and preindustrial spread is also
printed above panel <bold>(e)</bold>. Panel <bold>(f)</bold> and panel <bold>(g)</bold> are kernel density plots
estimating when the spring transition begins (PC1 <inline-formula><mml:math id="M29" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 0.5<inline-formula><mml:math id="M30" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>) and when
the spring transition ends (PC1 <inline-formula><mml:math id="M31" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> <inline-formula><mml:math id="M32" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.5<inline-formula><mml:math id="M33" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>), respectively.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/5101/2023/acp-23-5101-2023-f01.png"/>

        </fig>

      <p id="d1e704">The winter jet is present when PC1 <inline-formula><mml:math id="M34" display="inline"><mml:mi mathvariant="italic">&gt;</mml:mi></mml:math></inline-formula> 1 standard deviation
(<inline-formula><mml:math id="M35" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>), during which the Pacific jet is strong and narrow (Fig. 1a).
The spring jet is present when PC1 <inline-formula><mml:math id="M36" display="inline"><mml:mi mathvariant="italic">&lt;</mml:mi></mml:math></inline-formula> 0.5<inline-formula><mml:math id="M37" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M38" display="inline"><mml:mi mathvariant="italic">&gt;</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M39" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.5<inline-formula><mml:math id="M40" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>, at which point the subtropical jet weakens and shifts north,
and the secondary subtropical jet maximum extends between Hawaii and western
North America (Fig. 1b). The summer jet is present when PC1 <inline-formula><mml:math id="M41" display="inline"><mml:mi mathvariant="italic">&lt;</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M42" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1<inline-formula><mml:math id="M43" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> (Fig. 1c). The jet weakens substantially and remains shifted
poleward, and the secondary jet maximum over North America weakens. The
structure of winter, spring, and summer jets (Fig. 1a–c) compares well with
that from 1958–2017 Japanese Reanalysis-55 data (cf. Fig. 2, Breeden et al., 2021), as does the timing of the phase changes (Fig. 1d–g; cf. Figs. 1 and 3;
Breeden et al., 2021).</p>
      <p id="d1e778">The RCP8.5 North Pacific jet exhibits increases in variability compared to
the preindustrial control during much of spring and summer (Fig. 1e).
Recomputing Fig. 1e using EXP3, which includes RCP8.5 SSTs alone, confirms
that the changing jet variability is associated with the SSTs (not shown).
Despite these changes in variability, there is no statistically significant
change when the spring transition begins (Fig. 1f) or ends (Fig. 1g). The
start date for the preindustrial control (EXP1) is 31 March with a
<inline-formula><mml:math id="M44" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> of <inline-formula><mml:math id="M45" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">13</mml:mn></mml:mrow></mml:math></inline-formula> d, and the end date is 11 May <inline-formula><mml:math id="M46" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">8</mml:mn></mml:mrow></mml:math></inline-formula> d.
For the full RCP8.5 experiment (EXP2), the start date is 1 April   with
a <inline-formula><mml:math id="M47" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> of <inline-formula><mml:math id="M48" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:math></inline-formula> d, and the end date is 13 May  <inline-formula><mml:math id="M49" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">13</mml:mn></mml:mrow></mml:math></inline-formula> d. Consistent with Fig. 1g, the enhanced jet variability due to RCP8.5
conditions manifests as a broader distribution of end dates. With no robust
change in the timing of the spring transition, the calendar dates
corresponding to the late-winter, spring, and summer jet phases are similar
amongst the experiments. Therefore, in all subsequent figures, anomalies are
calculated by binning each individual experiment's data according to that
experiment's late-winter, spring, and summer days; time-averaging the data
within each bin; and then differencing between the jet phase (e.g., late
winter) bins from two different experiments (e.g., EXP2 minus EXP1). This
approach would not be possible if, for instance, the annually averaged late-winter end date from EXP2 was 10 d after that from the EXP1. Similar
results to those shown in Figs. 2–6 can be obtained by comparing like
months (e.g., February–March, April–May) from two different experiments (not
shown). However, we choose to show our results according to jet phase so
that the STT inherently associated with each phase is accounted for.</p>
      <p id="d1e836">Note that while no changes in the timing of the spring transition are found
in these simulations, spring transition timing is heavily influenced by the
El Niño–Southern Oscillation (ENSO; Breeden et al., 2021). Interannual
SST fluctuations (which may arise, for instance, due to ENSO) are excluded
from our experiments; hence, our results cannot comprehensively establish
how RCP8.5 forcing modifies the timing of the spring transition.</p>
</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>Residual advection, two-way isentropic mixing, production, and loss of
O3S</title>
      <?pagebreak page5105?><p id="d1e847">To quantify the contributions of the residual advection, two-way isentropic
mixing, and production and loss to the total O3S response, we calculate the
terms in the transformed Eulerian mean (TEM) continuity equation for zonal
mean tracer transport given by Andrews et al. (1987, Eq. 9.4.13) and
discussed by Abalos et al. (2013). Daily data, time-averaged from the
6-hourly fields, are used to calculate each term. These terms are shown in
Eq. (1):
            <disp-formula id="Ch1.E1" content-type="numbered"><label>1</label><mml:math id="M50" display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mo>∂</mml:mo><mml:mover accent="true"><mml:mi mathvariant="italic">χ</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mrow><mml:mrow><mml:mo>∂</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>+</mml:mo><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi>v</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mo>∂</mml:mo><mml:mover accent="true"><mml:mi mathvariant="italic">χ</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mrow><mml:mrow><mml:mo>∂</mml:mo><mml:mi>y</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>+</mml:mo><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi>w</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mo>∂</mml:mo><mml:mover accent="true"><mml:mi mathvariant="italic">χ</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mrow><mml:mrow><mml:mo>∂</mml:mo><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>P</mml:mi><mml:mo>-</mml:mo><mml:mi>L</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>+</mml:mo><mml:msup><mml:mi>e</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mi>z</mml:mi><mml:mo>/</mml:mo><mml:mi>H</mml:mi></mml:mrow></mml:msup><mml:mi mathvariant="normal">∇</mml:mi><mml:mo>⋅</mml:mo><mml:mi mathvariant="bold-italic">M</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
          where overbars denote zonal averages, <inline-formula><mml:math id="M51" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula> denotes the ozone
concentration in parts per billion, <inline-formula><mml:math id="M52" display="inline"><mml:mi>P</mml:mi></mml:math></inline-formula> denotes chemical production and <inline-formula><mml:math id="M53" display="inline"><mml:mi>L</mml:mi></mml:math></inline-formula>
chemical loss, <inline-formula><mml:math id="M54" display="inline"><mml:mi>H</mml:mi></mml:math></inline-formula> is the scale height equal to 7 km, <inline-formula><mml:math id="M55" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M56" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula>
are the meridional and zonal Cartesian coordinates, <inline-formula><mml:math id="M57" display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula> is log-pressure
height, <inline-formula><mml:math id="M58" display="inline"><mml:mi mathvariant="normal">∇</mml:mi></mml:math></inline-formula> is the divergence operator, and <inline-formula><mml:math id="M59" display="inline"><mml:mi>M</mml:mi></mml:math></inline-formula> is the two-way
isentropic mixing vector with meridional and vertical components given by
Eqs. (2) and (3):
<?xmltex \hack{\allowdisplaybreaks}?>

                <disp-formula specific-use="gather" content-type="numbered"><mml:math id="M60" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="Ch1.E2"><mml:mtd><mml:mtext>2</mml:mtext></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:msup><mml:mi mathvariant="bold-italic">M</mml:mi><mml:mi>y</mml:mi></mml:msup><mml:mo>=</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>-</mml:mo><mml:msup><mml:mi>e</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mfrac><mml:mi>z</mml:mi><mml:mi>H</mml:mi></mml:mfrac></mml:mrow></mml:msup><mml:mfenced open="(" close=")"><mml:mrow><mml:mi>v</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup><mml:mi mathvariant="italic">χ</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup><mml:mo>-</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mover accent="true"><mml:mrow><mml:mi>v</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup><mml:mi>T</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mi>S</mml:mi></mml:mfrac></mml:mstyle><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mo>∂</mml:mo><mml:mover accent="true"><mml:mi mathvariant="italic">χ</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mrow><mml:mrow><mml:mo>∂</mml:mo><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E3"><mml:mtd><mml:mtext>3</mml:mtext></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:msup><mml:mi mathvariant="bold-italic">M</mml:mi><mml:mi>z</mml:mi></mml:msup><mml:mo>=</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>-</mml:mo><mml:msup><mml:mi>e</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mfrac><mml:mi>z</mml:mi><mml:mi>H</mml:mi></mml:mfrac></mml:mrow></mml:msup><mml:mfenced close=")" open="("><mml:mrow><mml:mi>w</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup><mml:mi mathvariant="italic">χ</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup><mml:mo>+</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mover accent="true"><mml:mrow><mml:mi>v</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup><mml:mi>T</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mi>S</mml:mi></mml:mfrac></mml:mstyle><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mo>∂</mml:mo><mml:mover accent="true"><mml:mi mathvariant="italic">χ</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mrow><mml:mrow><mml:mo>∂</mml:mo><mml:mi>y</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

            where primes denote deviations from the zonal average, <inline-formula><mml:math id="M61" display="inline"><mml:mi>v</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M62" display="inline"><mml:mi>w</mml:mi></mml:math></inline-formula> are the
meridional and vertical velocities, <inline-formula><mml:math id="M63" display="inline"><mml:mi>S</mml:mi></mml:math></inline-formula> equals <inline-formula><mml:math id="M64" display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mi>H</mml:mi><mml:mo>⋅</mml:mo><mml:msup><mml:mi>N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>)</mml:mo><mml:mo>/</mml:mo><mml:mi>R</mml:mi></mml:mrow></mml:math></inline-formula> in which
<inline-formula><mml:math id="M65" display="inline"><mml:mrow><mml:msup><mml:mi>N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> is the Brunt–Väisälä frequency, and <inline-formula><mml:math id="M66" display="inline"><mml:mi>R</mml:mi></mml:math></inline-formula> is the gas
constant equal to 287 m<inline-formula><mml:math id="M67" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> s<inline-formula><mml:math id="M68" 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> K<inline-formula><mml:math id="M69" 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>. The residual circulation velocities
(<inline-formula><mml:math id="M70" display="inline"><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi>v</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:math></inline-formula>, <inline-formula><mml:math id="M71" display="inline"><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi>w</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:math></inline-formula>) are given by Eqs. (4) and (5):

                <disp-formula specific-use="gather" content-type="numbered"><mml:math id="M72" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="Ch1.E4"><mml:mtd><mml:mtext>4</mml:mtext></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi>v</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mo>=</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mover accent="true"><mml:mi>v</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mo>-</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mrow><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mo>∂</mml:mo><mml:mrow><mml:mo>∂</mml:mo><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mfenced open="(" close=")"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mover accent="true"><mml:mrow><mml:mi>v</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup><mml:mi mathvariant="italic">θ</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mrow><mml:mrow><mml:mo>∂</mml:mo><mml:mi mathvariant="italic">θ</mml:mi><mml:mo>/</mml:mo><mml:mo>∂</mml:mo><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mfenced></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E5"><mml:mtd><mml:mtext>5</mml:mtext></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi>w</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mo>=</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mover accent="true"><mml:mi>w</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mo>+</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mrow><mml:mi mathvariant="normal">acos</mml:mi><mml:mi mathvariant="italic">φ</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mo>∂</mml:mo><mml:mrow><mml:mo>∂</mml:mo><mml:mi mathvariant="italic">φ</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mfenced open="(" close=")"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi>cos⁡</mml:mi><mml:mi mathvariant="italic">φ</mml:mi><mml:mover accent="true"><mml:mrow><mml:mi>v</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup><mml:mi mathvariant="italic">θ</mml:mi><mml:msup><mml:mi/><mml:mo>′</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mrow><mml:mrow><mml:mo>∂</mml:mo><mml:mi mathvariant="italic">θ</mml:mi><mml:mo>/</mml:mo><mml:mo>∂</mml:mo><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mfenced><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

            where <inline-formula><mml:math id="M73" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ρ</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is log-pressure density, <inline-formula><mml:math id="M74" display="inline"><mml:mi mathvariant="italic">θ</mml:mi></mml:math></inline-formula> is potential
temperature, and <inline-formula><mml:math id="M75" display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula> is Earth's radius.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Results</title>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Lower-tropospheric O3S responses</title>
      <p id="d1e1529">To better understand how climate change may influence the amount of
stratospheric ozone making it into the lower free troposphere over western
North America, Fig. 2 shows the 700 hPa O3S responses to full RCP8.5
forcing, the change due to SSTs alone, and the change due to GHGs alone for
the late-winter, spring, and summer North Pacific jet phases. In the
preindustrial control climatology, lower-tropospheric O3S increases from low
to high latitudes regardless of season, and mixing ratios are largest over
the western North Pacific during the jet's spring phase, mimicking the observed
seasonal maximum in deep STT over this region (Fig. 2 black lines; Škerlak et al., 2014; Breeden et al., 2021).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2" specific-use="star"><?xmltex \currentcnt{2}?><?xmltex \def\figurename{Figure}?><label>Figure 2</label><caption><p id="d1e1534">The 700 hPa O3S (ppb) response to RCP8.5 boundary conditions shown in
shading. Panels <bold>(a)</bold>–<bold>(c)</bold> show the response to RCP8.5 conditions, panels <bold>(d)</bold>–<bold>(f)</bold> the response to
SSTs alone, and panels <bold>(g)</bold>–<bold>(i)</bold> the response to GHGs alone. The 700 hPa O3S preindustrial
control seasonal climatologies are overlaid in black. Non-stippled grid
points are statistically significant at a 5 % significance threshold using
a bootstrapping hypothesis test (Efron and Tibshirani, 1994) in which the two
samples being compared are resampled 1000 times at each grid point. The
phases of the jet are shown in successive columns. To identify by how much
700 hPa O3S changes over western North America compared to the preindustrial
control, spatial averages of the O3S anomalies were taken over the domain
boxed in Fig. 2a.</p></caption>
          <?xmltex \igopts{width=503.61378pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/5101/2023/acp-23-5101-2023-f02.png"/>

        </fig>

      <?pagebreak page5106?><p id="d1e1562"><?xmltex \hack{\newpage}?>RCP8.5 forcing increases lower-tropospheric O3S over most of the
longitudinal domain shown and over much of the hemisphere (not shown) during
all three seasons (Fig. 2a–c). The RCP8.5 response is largest in late
winter, during which there is up to a 50 % increase in O3S over the North
Pacific and a 37 % increase over western North America
(25–45<inline-formula><mml:math id="M76" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 235–260<inline-formula><mml:math id="M77" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E; Fig. 2a box). Although the responses are smaller
in absolute magnitude during spring and summer compared to winter, they
still imply roughly a 10 %–30 % change relative to climatology. Notably in
spring, the largest increases are centered over western North America (Fig. 2b).</p>
      <p id="d1e1585">The SSTs alone (Fig. 2d–f) increase O3S by approximately 15 % over the
eastern North Pacific during the jet's late-winter phase (Fig. 2d),
explaining a portion of the aforementioned 50 % increase in late winter
over this region due to full RCP8.5 forcing (cf. Fig. 2a). Over the low-latitude eastern North Pacific, close to Baja California, Mexico, the SSTs
alone promote large increases in O3S during the jet's winter and spring
phases relative to preindustrial climate (Fig. 2d–e). Conversely at high
latitudes, O3S does not change during the late-winter phase in response to
SSTs alone, and it decreases during both the jet's spring and summer phases.
In summary, the SSTs alone can explain a portion of the full RCP8.5
response but clearly not the bulk of it.</p>
      <p id="d1e1588">The response to GHGs alone accounts for the majority of the full RCP8.5 700 hPa O3S response (Fig. 2g–i). Larger O3S increases develop during the jet's
late-winter and spring phases compared to summer. Both SSTs alone and GHGs
alone increase O3S over the eastern North Pacific and western North America
during the jet's late-winter phase but have competing effects on O3S during
the jet's spring and summer phases. To better understand the future changes
in free tropospheric O3S and the relative roles of SST and GHG changes, the
next sections consider in more detail how the North Pacific jet and the
lower-stratospheric ozone reservoir respond to climate change.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e1593">As in Fig. 2 but for the 200 hPa zonal winds.</p></caption>
          <?xmltex \igopts{width=503.61378pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/5101/2023/acp-23-5101-2023-f03.png"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><title>Changes in the upper troposphere and lower stratosphere</title>
      <p id="d1e1610">RCP8.5 conditions accelerate, narrow, and elongate the late-winter North
Pacific jet towards western North America at 200 hPa (Fig. 3a). This change
is robust to varying severities of climate change (RCP4.5, Harvey et al., 2020; RCP6.0, Akritidis et al., 2019; and RCP8.5, Matsumura et al., 2021).
Contrary to what takes place during the late-winter period, the subtropical
jet shifts equatorward during the jet's spring and summer phases (Fig. 3b–c). At lower latitudes, westerly anomalies form over the subtropical
eastern Pacific and<?pagebreak page5107?> central America, where there is a climatological minimum in
the 200 hPa zonal wind (Fig. 3a–c). This response is present during all
three jet phases and strengthens from late winter through summer (Fig. 3a–c).</p>
      <p id="d1e1613">The full RCP8.5 200 hPa zonal wind response is dominated by the contribution
from the SSTs alone (Fig. 3d–f), with the GHGs alone (Fig. 3g–i) playing a
comparatively minor role. The strong influence of the SSTs on the wind
response arises in part because the SST forcing is associated with almost
all of the <inline-formula><mml:math id="M78" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 9–11 K warming of the tropical upper
troposphere and the amplified Arctic surface warming (Fig. S1) and so
dominates the influence on meridional temperature gradients and associated
circulation changes that drive heat transport. Another consideration is that
the zonal asymmetries in the pattern of SSTs prescribed in the experiments,
particularly those over the tropical Pacific resembling El Niño (Fig. S2), may elicit teleconnections (e.g., Pacific North America (PNA)
teleconnection pattern) that modify the upper-tropospheric circulation. In
general, the impact of the GHGs alone on the 200 hPa winds is small,
although the GHGs alone do have a large (compared to climatology) effect on
the zonal wind over western North America during the jet's summer phase
(Fig. 3i), illustrating that purely chemical changes in the stratosphere are
capable of having significant dynamical impacts.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e1625">The 200 hPa O3S (shaded, ppb) and stationary wave (“GEOPx”),
visualized by geopotential height deviation from its long-term monthly zonal
mean (contours, meters), responses to RCP8.5 boundary conditions. Panels <bold>(a)</bold>–<bold>(c)</bold> show
the preindustrial climatologies of O3S in alternate shading and the
climatological stationary wave in contours <bold>(d)</bold>–<bold>(l)</bold>. Panels <bold>(d)</bold>–<bold>(f)</bold> show O3S response to
RCP8.5 conditions in shading and stationary wave anomalies as contours,
panels <bold>(g)</bold>–<bold>(i)</bold> the same but for SSTs alone, and panels <bold>(j)</bold>–<bold>(l)</bold> the same but for GHGs alone.
Non-stippled grid points are statistically significant O3S anomalies at a
5 % significance threshold using a bootstrapping hypothesis test. The
phases of the jet are shown in successive columns. The preindustrial control
thermal tropopauses for each season are shown in cyan, and anomalous
tropopauses are shown in blue.</p></caption>
          <?xmltex \igopts{width=503.61378pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/5101/2023/acp-23-5101-2023-f04.png"/>

        </fig>

      <p id="d1e1666">Figure 4 shows how RCP8.5 conditions modify 200 hPa O3S, allowing us to see
both tropospheric and stratospheric ozone changes; at 200 hPa, the
stratosphere is poleward of the anomalous thermal tropopause (blue lines),
which can be compared with the preindustrial thermal tropopause (cyan lines)
in each season. The 200 hPa O3S equatorward of the tropopause has already
been transported into the troposphere and can be lost due to dry deposition, photolysis, and chemical loss or transported back to the stratosphere by
reversible mixing processes.</p>
      <p id="d1e1669">In the preindustrial control (EXP1), O3S maxima and minima are co-located
with the troughs and ridges of the climatological stationary wave (Fig. 4a–c). This is particularly clear in late winter, during which O3S mixing
ratios exceed 600 ppb over the wave-1-scale trough of the climatological
stationary wave, the Aleutian Low (Fig. 4a). O3S mixing ratios are, on the
other hand, reduced over the climatological Alaskan ridge. Slightly out of
view in Fig. 4a is a climatological wave-2-scale trough that resides over the
Baffin Bay and Greenland; an O3S maximum is found over this region as well
(Fig. 4a). As suggested by Reed (1950; see also Schoeberl and Kreuger, 1983; Salby and Callaghan, 1993), horizontal advection and vertical motion
associated with waves act to concentrate ozone in troughs and reduce it over
ridges. The climatological stationary wave influences the 200 hPa
composition of O3S in this way.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><?xmltex \currentcnt{5}?><?xmltex \def\figurename{Figure}?><label>Figure 5</label><caption><p id="d1e1674">Transects of the O3S anomalies and isentropes averaged between
235  and 260<inline-formula><mml:math id="M79" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E (over western North America). Panels <bold>(a)</bold>–<bold>(c)</bold>
show preindustrial climatologies of O3S; contour intervals are 20, 40, 60,
80, 100, 200, 500 (shown by thick black contour), 1000, 2000, 3000, and 4000 ppb. Panels <bold>(d)</bold>–<bold>(f)</bold> show O3S response to RCP8.5 forcing in shading, with
preindustrial isentropes shown in black and the anomalous isentropes in
magenta; panels <bold>(g)</bold>–<bold>(i)</bold> show the same but for SSTs alone and panels <bold>(j)</bold>–<bold>(l)</bold> the same but for
GHGs alone. Non-stippled grid points are statistically significant O3S
responses at a 5 % significance threshold using a bootstrapping hypothesis
test. The phases of the jet are shown in successive columns.</p></caption>
          <?xmltex \igopts{width=503.61378pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/5101/2023/acp-23-5101-2023-f05.png"/>

        </fig>

      <p id="d1e1717">Full RCP8.5 conditions increase lower-stratospheric O3S over much of the
hemisphere during all seasons (Fig. 4d–f). The largest regional increase is
a doubling of O3S over the North Pacific during the jet's late-winter phase
(Fig. 4a, d). This regional O3S increase is co-located with the trough of
an anomalous tropical–extratropical planetary-scale wave, whose signature is
apparent in the zonal wind response (Fig. 3) and the stationary wave
response (Fig. 4, black contours). As the amplitude of this wave diminishes
during the<?pagebreak page5108?> spring and summer phases, so does the lower-stratospheric O3S
maximum (Fig. 4e–f). The RCP8.5 O3S response is mostly contained in the lower-stratospheric (i.e., poleward of the tropopause) trough during the jet's
late-winter phase, but in the absence of strong meridional potential
vorticity gradients such as the high-latitude polar stratospheric westerlies
(Manney et al., 1994; Salby and Callaghan, 2007) or the subtropical jet stream
(Bönisch et al., 2009), which serve as transport barriers, the O3S
response “smears out” during spring and summer, becoming more evenly
distributed around the 200 hPa thermal tropopause (Fig. 4e–f).</p>
      <p id="d1e1720">The SSTs alone are almost solely responsible for the development of the
anomalous planetary wave and are therefore a key reason why there are zonal
asymmetries in the lower-stratospheric ozone reservoir (Fig. 4g–i). Similar
effects of large-scale planetary wave trains on lower-stratospheric ozone
have been noted in relation to ENSO (Zhang et al., 2015; Albers et al., 2022).
The SST forcing considered in this study displays SST warming globally but
contains some zonal asymmetries, one of them being an El Niño-like
eastern tropical Pacific warming (Fig. S2). This zonal asymmetry may explain
why the planetary wave response to the SSTs alone during late winter (Fig. 4g) resembles the PNA wave train known to develop with El Niño (albeit
the Canadian ridge in Fig. 4g is displaced east relative to the PNA Canadian
ridge). Note though that there is large inter-model and inter-generational
(CMIP5 vs. CMIP6) spread in how ENSO responds to climate change
(Beobide-Arsuga et al., 2021; Cai et al., 2022), suggesting that this
planetary wave response could vary amongst climate models should it in fact
be related to the El Niño-like warming superimposed on the global SST
increase (Fig. S2).</p>
      <?pagebreak page5109?><p id="d1e1724">Contrary to the SSTs alone, the GHGs alone have little effect on the
planetary-scale eddies and elicit more zonally symmetric O3S responses (Fig. 4j–l). The lower-stratospheric O3S response to the GHGs alone develops
largely due to net chemical production of stratospheric ozone, likely
associated with the large methane increase in RCP8.5, which enhances O<inline-formula><mml:math id="M80" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
mixing ratios in the extratropical stratosphere (Morgenstern et al., 2018),
and changes in transport associated with the BDC's deep branch.</p>
      <p id="d1e1736">To further clarify how the lower-stratospheric reservoir responds to RCP8.5
conditions, Fig. 5 shows latitude–pressure transects of O3S anomalies and
isentropes averaged between 235 and 260<inline-formula><mml:math id="M81" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E (over
western North America; the same longitudinal bounds used for the box in Fig. 2a).
Climatologically, extratropical lower-stratospheric O3S mixing ratios are
larger during winter and spring (Fig. 5b), following from transport by the
BDC's deep branch (Ray et al., 1999; Hegglin and Shepherd, 2007; Bönisch
et al., 2009; Butchart, 2014; Konopka et al., 2015; Ploeger and Birner, 2016;
Albers et al., 2018). During summer in climatology, enhanced isentropic
mixing between the tropical and extratropical lowermost stratosphere
(Hegglin and Shepherd, 2007; Abalos et al., 2013) and rising tropopause
heights (Schoeberl et al., 2004) act to flush ozone out of the lowermost
stratosphere.</p>
      <p id="d1e1748">During every jet phase, RCP8.5 conditions reduce O3S in the low-latitude
stratosphere while promoting accumulation of O3S at high latitudes (Fig. 5d–f). Some of this O3S accumulating in the extratropical lower stratosphere
may enter the troposphere along the subtropical upper-tropospheric and lower-stratospheric isentropes (e.g., 360 K). Both the GHGs alone and SSTs alone
play a role in making this happen. The upper-tropospheric warming induced by
the SSTs alone depresses the isentropes (e.g., 360 K) to lower altitudes,
enhancing the access of the troposphere to lower-stratospheric air (Fig. 5g–i), where wave breaking is able to transport the ozone into the
subtropical and tropical upper troposphere (e.g., Waugh and Polvani, 2000;
Albers et al., 2016, and references therein). The GHGs alone on the other hand
mainly contribute by more broadly enhancing the extratropical lower-stratospheric O3S concentrations (Fig. 5j–l).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><?xmltex \currentcnt{6}?><?xmltex \def\figurename{Figure}?><label>Figure 6</label><caption><p id="d1e1753">Residual advective O3S tendencies (shading) and residual mass
streamfunction (contours). Panels <bold>(a)</bold>–<bold>(c)</bold> show preindustrial residual advective O3S
tendencies in shading, with the climatological residual mass streamfunction
overlaid in black contours. The color scale is the same for the climatology
and anomalies. The contour intervals for the residual mass streamfunction in
all panels are 0.025, 0.05, 0.1, 0.25, 0.5, 1, 5, 10, 15, 20, 25, etc. (<inline-formula><mml:math id="M82" display="inline"><mml:mrow><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">9</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> kg s<inline-formula><mml:math id="M83" 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>). Panels <bold>(d)</bold>–<bold>(f)</bold> show the O3S tendency and
streamfunction anomalies to RCP8.5; panels <bold>(g)</bold>–<bold>(i)</bold> show the same but for SSTs alone
and panels <bold>(j)</bold>–<bold>(l)</bold> the same but for GHGs alone. Non-gray shaded grid points show
statistically significant O3S tendency anomalies at a 5 % significance
threshold using a bootstrapping hypothesis test. The phases of the jet are
shown in successive columns. For each phase of the jet, the preindustrial
control thermal tropopause is black, and the anomalous tropopause is gray.
Note that an anomalous tropopause is hardly visible in response to GHGs
alone, as the SSTs alone are the forcing that modifies the tropopause.</p></caption>
          <?xmltex \igopts{width=503.61378pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/5101/2023/acp-23-5101-2023-f06.png"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><?xmltex \currentcnt{7}?><?xmltex \def\figurename{Figure}?><label>Figure 7</label><caption><p id="d1e1812">Two-way isentropic mixing O3S tendencies (shading) and zonal mean
zonal wind (contours). Panels <bold>(a)</bold>–<bold>(c)</bold> show preindustrial O3S tendencies in shading,
with the climatological zonal wind overlaid in black (<inline-formula><mml:math id="M84" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> m s<inline-formula><mml:math id="M85" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>), and the
components of the two-way isentropic mixing (<inline-formula><mml:math id="M86" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="bold-italic">M</mml:mi><mml:mi>y</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M87" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="bold-italic">M</mml:mi><mml:mi>z</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) shown as vectors. The
color scale is the same for the climatology and anomalies. Panels <bold>(d)</bold>–<bold>(f)</bold> show the
O3S tendency and zonal wind anomalies to RCP8.5; panels <bold>(g)</bold>–<bold>(i)</bold> show the same but
for SSTs alone and panels <bold>(j)</bold>–<bold>(l)</bold> the same but for GHGs alone. Non-gray shaded grid
points show statistically significant O3S anomalies at a 5 % significance
threshold using a bootstrapping hypothesis test. The phases of the jet are
shown in successive columns. For each phase of the jet, the preindustrial
control thermal tropopause is black, and the anomalous tropopause is gray.</p></caption>
          <?xmltex \igopts{width=503.61378pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/5101/2023/acp-23-5101-2023-f07.png"/>

        </fig>

      <p id="d1e1896">O3S is reduced near the extratropical tropopause in all seasons in response
to RCP8.5 forcing (Fig. 5d–f). This is associated with the increased height
of the tropopause (Abalos et al., 2017) resulting from the SSTs alone. Due to
steep vertical gradients in tracers near the tropopause (e.g., Pan et al., 2004), taking the difference between an experiment with a lifted tropopause
(EXP2 or EXP3) and an experiment without this feature (preindustrial
control, EXP1) amounts to taking the difference between relatively O3S-depleted tropospheric air and O3S-rich stratospheric air; hence, the negative
O3S anomalies develop near the tropopause (Fig. 5d–i). This negative O3S
response can largely be removed by remapping the vertical axis of each data
field used to make, for instance, Fig. 5d–f (zonally averaged RCP8.5 (EXP2)
O3S and preindustrial (EXP1) O3S) to tropopause-relative coordinates (meters
above or below the thermal tropopause), then taking the difference between
these two modified data fields and remapping this set of anomalies (axes:
tropopause-relative <inline-formula><mml:math id="M88" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> latitude) to a log-pressure coordinate system (axes:
pressure <inline-formula><mml:math id="M89" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> latitude) (Abalos et al., 2017). Using annual cycles of thermal
tropopause and O3S data, which should help to smooth out the large
hourly/daily fluctuations in these fields near the tropopause, the
aforementioned procedure was applied to a zonally averaged transect over the
North Pacific (Fig. S3) and applied at all grid points at 200 hPa (Fig. S4)
and 300 hPa (Fig. S5). While this tropopause-relative analysis does remove
the majority of the negative O3S response associated with the tropopause
lift, the strong O3S zonal asymmetries associated with the planetary wave
response to the SSTs alone persist, namely the negative O3S response
corresponding to the planetary wave's ridge near Alaska (cf. Figs. 4k, S5e). This analysis corroborates that the higher<?pagebreak page5111?> tropopause in RCP8.5 is
largely responsible for the presence of the negative O3S response in the
extratropical upper troposphere and lower stratosphere, however, not entirely, as
we find that a portion of this negative O3S is associated with the anomalous
planetary wave's zonally asymmetric effects on the upper-tropospheric and lower-stratospheric O3S distribution.</p>
</sec>
<sec id="Ch1.S3.SS3">
  <label>3.3</label><title>Zonally symmetric changes</title>
      <p id="d1e1921">The seasonal variability of both tropical (Abalos et al., 2013) and
extratropical (Albers et al., 2018) lower-stratospheric ozone tendencies is
heavily influenced by upwelling and downwelling associated with BDC's
residual mean meridional circulation component. This circulation is made up
of a shallow and a deep branch. Transport associated with the shallow branch
proceeds more horizontally, and the air masses enter the stratosphere closer
to the subtropics, whereas transport associated with the deep branch is more
vertical, and the air masses enter the stratosphere through the deep tropics
and descend at high latitudes (Birner and Bönisch, 2011). To quantify the
influence of RCP8.5 forcing on these physical processes, Fig. 6 shows the
residual mass streamfunction response to RCP8.5 forcing in black contours
and in shading the local changes in O3S tendencies as a result of transport
by the residual mean meridional circulation terms in the TEM continuity
equation (<inline-formula><mml:math id="M90" display="inline"><mml:mrow><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi>v</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow><mml:mo>∂</mml:mo><mml:mover accent="true"><mml:mi mathvariant="italic">χ</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mrow><mml:mrow><mml:mo>∂</mml:mo><mml:mi>y</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>+</mml:mo><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi>w</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow><mml:mo>∂</mml:mo><mml:mover accent="true"><mml:mi mathvariant="italic">χ</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mrow><mml:mrow><mml:mo>∂</mml:mo><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:math></inline-formula>). As in
reanalysis (cf. Rosenlof, 1995), in the preindustrial control, the tropical
upward mass flux peaks in amplitude during boreal winter when the residual
mass streamfunction is<?pagebreak page5112?> strongest (Fig. 6a). As the zonal momentum budget
changes in each hemisphere during spring and summer, the tropical upward
mass flux shifts into the Northern Hemisphere, and the residual mass
streamfunction weakens and shifts downward towards the troposphere (Fig. 6b,
c). The negative O3S tendencies in the tropical lower stratosphere track the
latitudinal shifting of the tropical upward mass flux over time. The
positive O3S tendencies in the extratropical lower stratosphere associated
with poleward transport of stratospheric ozone from its tropical source
region peak in amplitude during winter when the BDC's deep branch is
strongest and weaken thereafter.</p>
      <p id="d1e1981">RCP8.5 forcing strengthens the shallow branch of the BDC during all three
seasons, reducing tropical stratospheric O3S tendencies (Fig. 6d–f). The
SSTs alone (Fig. 6g–i) are primarily responsible for the acceleration of the
residual mass streamfunction in the subtropical lower stratosphere (50 hPa/30<inline-formula><mml:math id="M91" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) when compared against the GHGs alone (Fig. 6j–l),
consistent with Oberländer et al. (2013) and Chrysanthou et al., (2020).
The upper component of the Hadley circulation near 150 hPa and 15<inline-formula><mml:math id="M92" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N accelerates, as previously reported by Abalos et al. (2020). All models that
they studied included this response. This feature acts cooperatively with
the reinforced BDC shallow branch to increase O3S transport through the
subtropical tropopause into the upper troposphere (200 hPa and 30<inline-formula><mml:math id="M93" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), with the largest increase occurring during summer in response to the
SSTs alone (Fig. 6i). The GHGs alone accelerate the deep branch well above
30 hPa during winter (Fig. 6j); the deep branch's high-latitude downwelling increases
lower-stratospheric O3S during spring (Fig. 6k) and then disappears by
summer (Fig. 6i).</p>
      <p id="d1e2011">Another aspect of the BDC is two-way isentropic mixing, which
climatologically increases subtropical O3S tendencies above and south of the
subtropical jet, while reducing extratropical O3S tendencies throughout the
stratosphere (Fig. 7a–c). In the tropical lower stratosphere
(<inline-formula><mml:math id="M94" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> 80 hPa), tendencies peak during summer in present-day
analyses (Abalos et al., 2013) and in the preindustrial control climatology
(Fig. 7c). RCP8.5 forcing generally reinforces the climatological two-way
isentropic mixing in the stratosphere during each season, increasing
subtropical tendencies and reducing extratropical tendencies (Fig. 7d–f).
Additionally, enhanced cross-tropopause mixing by eddies increases upper-tropospheric O3S tendencies from 30–60<inline-formula><mml:math id="M95" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, with stronger signals during summer
than winter. These anomalies are primarily associated with the SSTs alone
(Fig. 7g–i). Hardly any part of the two-way isentropic mixing responses to
GHGs alone are statistically significant (Fig. 7j–l).</p>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <label>4</label><title>Conclusions</title>
      <p id="d1e2039">We use three interactive-chemistry WACCM experiments to analyze how
stratosphere-to-troposphere transport of ozone over western North America
during late winter, spring, and summer responds to worst-case scenario
RCP8.5 climate change at the end of the century. Lower-tropospheric O3S
concentrations increase up to 37 % during late winter over western North
America in response to RCP8.5 forcing, with progressively weaker increases
during spring and summer. Between the GHGs alone and SSTs alone, the GHGs
alone are found to be primarily responsible for increase in lower-tropospheric O3S over western North America and across the Northern
Hemisphere.</p>
      <p id="d1e2042">Because lower-stratospheric ozone mixing ratios are positively correlated
with the amount of ozone contained in intrusions that transport mass into
the troposphere (Ordóñez et al., 2007; Hess and Zbinden, 2013; Neu et al., 2014; Albers et al., 2016, 2018), we document the processes modifying
future lower-stratospheric ozone. The portion of the full RCP8.5 response
driven by the GHGs alone (no changes to the SSTs) promotes higher ozone
mixing ratios throughout the extratropical lower stratosphere. It is
unlikely that these increases are associated with dynamical changes due to
GHGs alone. In agreement with Oberländer et al. (2013) and Chrysanthou
et al. (2020), we find that the GHGs alone modify residual advective
transport, promoting some increases in extratropical lower-stratospheric
ozone. However, this response, in combination with the weak eddy transport
response to the GHGs alone, cannot wholly explain the changes in
extratropical lower-stratospheric O3S that occur during winter, spring, and
summer due to GHGs; thus, we conclude that production of ozone must be an
important component of the response to GHGs. Note that different GHGs have
unique chemical influences on ozone (e.g., Fleming et al., 2011), which we do
not attempt to separate in this study (see Morgenstern et al., 2018). We
hypothesize that the higher tropospheric O3S driven by GHGs alone is
associated with enhanced production of ozone throughout the extratropical
lower stratosphere, likely due to 4.6 times higher methane concentrations in the
RCP8.5 experiment compared to the preindustrial control (Portmann and Solomon,
2007; Revell et al., 2012; Morgenstern et al., 2018; Winterstein et al., 2019).
The ozone increases evidently outweigh any ozone reductions forced by the
1.5 times and 3 times increases in N<inline-formula><mml:math id="M96" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>O and Cl<inline-formula><mml:math id="M97" display="inline"><mml:msub><mml:mi/><mml:mi>y</mml:mi></mml:msub></mml:math></inline-formula>, respectively, culminating in
a net ozone increase throughout the extratropical lower stratosphere (Fig. 5j–k).</p>
      <p id="d1e2063">The SSTs alone promote scattered regional increases and decreases in lower-tropospheric O3S. Over the North Pacific, the lower-tropospheric O3S
increases are co-located with the low-pressure center of the largest
anomalous trough of a tropics–extratropics planetary-scale wave that forms
over the North Pacific, similar to the PNA wave train, in response to the
SSTs alone. When the amplitude of this wave is largest (during late winter),
O3S increases by nearly 400 ppb within the wave's largest trough at 200 hPa,
a doubling of O3S relative to the preindustrial control climatology. A large
part of this trough is located in the lower stratosphere at 200 hPa,
illustrating that planetary waves can introduce high-amplitude<?pagebreak page5113?> zonal
asymmetries into the lower-stratospheric ozone reservoir that then
coincide with regionally enhanced STT. In agreement with Reed (1950), we
attribute the co-location between lower-stratospheric troughs (ridges) and
enhanced (reduced) ozone to horizontal advection and vertical motion induced
by the North Pacific planetary-scale wave. Although their studies focus on
ENSO, Zhang et al. (2015) and Albers et al. (2022) each provide more
detailed observational and model-based evidence in favor of this physical
mechanism.</p>
      <p id="d1e2066">One interesting result is that the quasi-zonally symmetric increase in lower
extratropical stratospheric ozone due to the GHGs alone (Fig. 4j–k) mirrors
the quasi-zonally symmetric increase in lower-tropospheric O3S below it
(Fig. 2j–k). Similarly, the highly regional changes in lower extratropical
stratospheric ozone forced by the SSTs alone (Fig. 4g–i) are co-located to, but
above, the regional changes in lower-tropospheric O3S forced by the SSTs
alone (Fig. 2g–i). Taken together, these results suggest that the spatial
distribution of ozone in the lower-stratospheric reservoir informs the
spatial distribution of lower-tropospheric O3S responses; similar
conclusions may be drawn from Albers et al. (2022; cf. their Figs. 4 and
8).</p>
      <p id="d1e2070">The SSTs alone are found to increase the year-to-year variability of the
North Pacific jet's seasonal evolution, particularly during spring and
summer, broadening the distribution of days on which the spring transition
may end, which in theory could coincide with more erratic year-to-year
fluctuations in STT of ozone in the future. Despite this, we find no
statistically significant change in the timing of the spring transition in
response to full RCP8.5 forcing. Since the experiments use fixed repeating
annual cycles of sea surface temperature and therefore exclude interannual
SST fluctuations, which are known to modify the seasonal variability of the
North Pacific jet (Langford, 1999; Zhang et al., 2015; Breeden et al., 2021;
Albers et al., 2022), our results cannot be used to comprehensively establish
whether or not the seasonal variability of the North Pacific jet,
particularly its spring transition, will change in response to climate
change. Our results do, however, illustrate that changes in SSTs have a strong
effect on the North Pacific jet, and in general, the SSTs alone account for
the majority of changes to the large-scale atmospheric circulation in the
full RCP8.5 forcing. For example, the SSTs alone drive the acceleration and
elongation of the late-winter North Pacific jet, the equatorward shift of
the spring and summer North Pacific jet, the acceleration of the BDC's
shallow branch, some of the deep branch acceleration, and most of the
two-way isentropic mixing responses. Considering that the SSTs alone
account for many of the changes to the large atmospheric circulation, an
avenue for future research is to analyze inter-model spread in the future
residual mean circulation response (Oman et al., 2010; Butchart, 2014; Abalos
et al., 2021) and the two-way isentropic mixing response (Eichinger et al., 2019; Abalos et al., 2020) as a function of inter-model spread in future
SSTs.</p>
      <p id="d1e2073">Given that the response to GHGs alone accounts for the majority of the full
RCP8.5 lower-tropospheric O3S response over western North America, it is
interesting to consider how a different climate change scenario may impact
our tropospheric O3S responses. Future STT exhibits large inter-scenario
spread (Young et al., 2013). Considering that RCP4.5, RCP6.0, and RCP8.5 use
equivalent Cl<inline-formula><mml:math id="M98" display="inline"><mml:msub><mml:mi/><mml:mi>y</mml:mi></mml:msub></mml:math></inline-formula> emissions (Meinshausen et al., 2011), it seems more
likely that the results herein would change due to the different
concentrations of CH<inline-formula><mml:math id="M99" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:math></inline-formula>, N<inline-formula><mml:math id="M100" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>O, and CO<inline-formula><mml:math id="M101" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> prescribed under the
other scenarios, as opposed to the Cl<inline-formula><mml:math id="M102" display="inline"><mml:msub><mml:mi/><mml:mi>y</mml:mi></mml:msub></mml:math></inline-formula>. In particular, lower
concentrations of CH<inline-formula><mml:math id="M103" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:math></inline-formula> would likely coincide with a smaller net increase
in extratropical lower-stratospheric ozone (e.g., Revell et al., 2012) and
therefore reduced STT of ozone over western North America. Indeed,
tropospheric column ozone decreases by the end of the century under RCP2.6
and RCP4.5 but increases due to RCP8.5 conditions (Archibald et al., 2020),
although to be clear, many factors (e.g., ozone precursors, Young et al., 2013) and not just STT will influence future tropospheric ozone. A
different climate change scenario would also produce a different dynamical
response to climate change; for instance, the strength of the BDC shallow
branch response to climate change scales with the change in future tropical
surface temperature warming (Abalos et al., 2021) and the change in future
global SSTs (Chrysanthou et al., 2020). This suggests that a different
climate change scenario would beget a different planetary wave response over
the North Pacific and, hence, different regional STT responses. For climate
change scenarios with weaker radiative forcing change and presumably less
production of extratropical lower-stratospheric ozone, the dynamical
response to the SSTs alone under these scenarios may play a more important
role in influencing STT of ozone than we find herein with the RCP8.5
scenario.</p>
</sec>

      
      </body>
    <back><notes notes-type="codedataavailability"><title>Code and data availability</title>

      <p id="d1e2136">The code used to perform this analysis can be accessed by personal
communication with the corresponding author. The WACCM simulation data used
to create the figures can be accessed here:
<uri>https://csl.noaa.gov/groups/csl8/modeldata/data/Elsbury_etal_2022/</uri> (NOAA, 2022).</p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d1e2142">The supplement related to this article is available online at: <inline-supplementary-material xlink:href="https://doi.org/10.5194/acp-23-5101-2023-supplement" xlink:title="pdf">https://doi.org/10.5194/acp-23-5101-2023-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e2151">DE wrote the code to do the analyses, created the figures, and wrote the
paper. AHB ran the climate model experiments. AHB, JRA, MLB, and AO'NL
edited and provided comments on the paper.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e2157">The contact author has declared that none of the authors has any competing interests.</p>
  </notes><notes notes-type="disclaimer"><title>Disclaimer</title>

      <p id="d1e2163">Publisher’s note: Copernicus Publications remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e2169">The authors would like to thank two anonymous reviewers for their thoughtful and constructive comments.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e2174">John R. Albers and Dillon Elsbury were funded in part by the National Science
Foundation (grant no. 1756958). Dillon Elsbury, John R. Albers, and Melissa L. Breeden were supported in part by NOAA (cooperative agreement nos. NA17OAR4320101 and NA22OAR4320151).</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e2180">This paper was edited by Marc von Hobe and reviewed by two anonymous referees.</p>
  </notes><ref-list>
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