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  <front>
    <journal-meta>
<journal-id journal-id-type="publisher">ACP</journal-id>
<journal-title-group>
<journal-title>Atmospheric Chemistry and Physics</journal-title>
<abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title>
<abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys.</abbrev-journal-title>
</journal-title-group>
<issn pub-type="epub">1680-7324</issn>
<publisher><publisher-name>Copernicus GmbH</publisher-name>
<publisher-loc>Göttingen, Germany</publisher-loc>
</publisher>
</journal-meta>

    <article-meta>
      <article-id pub-id-type="doi">10.5194/acp-15-11461-2015</article-id><title-group><article-title>The impacts of volcanic aerosol on stratospheric ozone
and the Northern Hemisphere polar vortex: separating radiative-dynamical
changes from direct effects due to enhanced aerosol heterogeneous chemistry</article-title>
      </title-group><?xmltex \runningtitle{Ozone response to volcanic eruption}?><?xmltex \runningauthor{S.~Muthers et~al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1 aff2">
          <name><surname>Muthers</surname><given-names>S.</given-names></name>
          <email>muthers@climate.unibe.ch</email>
        <ext-link>https://orcid.org/0000-0002-3691-4387</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Arfeuille</surname><given-names>F.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Raible</surname><given-names>C. C.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4 aff5">
          <name><surname>Rozanov</surname><given-names>E.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-0479-4488</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Climate and Environmental Physics, University of Bern, Bern, Switzerland</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Oeschger Centre for Climate Change Research, University of Bern, Bern, Switzerland</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Suisse Federal Laboratories for Material Science and Technology (Empa) Duebendorf, Switzerland</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Institute for Atmospheric and Climate Science, ETH, Zurich, Switzerland</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>Physikalisch-Meteorologisches Observatorium Davos and World  Radiation Center (PMOD/WRC), Davos, Switzerland</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">S. Muthers (muthers@climate.unibe.ch)</corresp></author-notes><pub-date><day>16</day><month>October</month><year>2015</year></pub-date>
      
      <volume>15</volume>
      <issue>20</issue>
      <fpage>11461</fpage><lpage>11476</lpage>
      <history>
        <date date-type="received"><day>30</day><month>March</month><year>2015</year></date>
           <date date-type="rev-request"><day>20</day><month>May</month><year>2015</year></date>
           <date date-type="rev-recd"><day>30</day><month>August</month><year>2015</year></date>
           <date date-type="accepted"><day>10</day><month>September</month><year>2015</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>After major volcanic eruptions the enhanced aerosol causes ozone changes due
to greater heterogeneous chemistry on the particle surfaces (HET-AER) and
from dynamical effects related to the radiative heating of the lower
stratosphere (RAD-DYN). We carry out a series of experiments with an
atmosphere–ocean–chemistry–climate model to assess how these two processes
change stratospheric ozone and Northern Hemispheric (NH) polar vortex
dynamics. Ensemble simulations are performed under present day and
preindustrial conditions, and with aerosol forcings representative of
different eruption strength, to investigate changes in the response
behaviour. We show that the halogen component of the HET-AER effect dominates
under present-day conditions with a global reduction of ozone
(<inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>21 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">DU</mml:mi></mml:math></inline-formula> for the strongest eruption) particularly at high latitudes,
whereas the HET-AER effect increases stratospheric ozone due to <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">5</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>
hydrolysis in a preindustrial atmosphere (maximum anomalies <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>4 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">DU</mml:mi></mml:math></inline-formula>).
The halogen-induced ozone changes in the present-day atmosphere offset part
of the strengthening of the NH polar vortex during mid-winter (reduction of
up to <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>16 <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> in January) and slightly amplify the dynamical
changes in the polar stratosphere in late winter (<inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>11 <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> in
March). The RAD-DYN mechanism leads to positive column ozone anomalies which
are reduced in a present-day atmosphere by amplified polar ozone depletion
(maximum anomalies <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>12 and <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>18 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">DU</mml:mi></mml:math></inline-formula> for present day and
preindustrial, respectively). For preindustrial conditions, the ozone
response is consequently dominated by RAD-DYN processes, while under present-day conditions, HET-AER effects dominate. The dynamical response of the
stratosphere is dominated by the RAD-DYN mechanism showing an intensification
of the NH polar vortex in winter (up to <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>10 <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> in January).
Ozone changes due to the RAD-DYN mechanism slightly reduce the response of
the polar vortex after the eruption under present-day conditions.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p>Tropical eruptions strong enough to inject into the
stratosphere perturb the physical and the chemical states of the climate
system for several years and longer
<xref ref-type="bibr" rid="bib1.bibx48 bib1.bibx18 bib1.bibx67" id="paren.1"/>. Although a range of gases are
injected <xref ref-type="bibr" rid="bib1.bibx64" id="paren.2"><named-content content-type="pre">e.g.</named-content></xref>, the global climate impacts stem from the
aerosol produced from the injected sulfur dioxide (<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>). In the
stratosphere volcanically injected <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is converted into sulfuric
acid (<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>) aerosols that (i) reflect in the visible part of
the solar spectrum, (ii) absorb terrestrial and solar infrared radiation, and
(iii) provide surface for a large number of chemical reactions that alter the
chemical composition of the stratosphere <xref ref-type="bibr" rid="bib1.bibx27" id="paren.3"/>. The enhanced
stratospheric aerosol increases the optical depth of the atmosphere, leading
to a decrease in SW radiation in the troposphere and at the surface.
Increased absorption of long wave and solar near-infrared radiation increases
heating rates in the volcanic plume causing a pronounced warming of the
tropical stratosphere. The perturbed vertical and meridional temperature
gradients alter the stratospheric circulation and via interaction between the
stratosphere and the troposphere affect surface climate. A prominent example
for this mechanism is the winter warming pattern in the NH observed after
several large tropical volcanic eruptions
<xref ref-type="bibr" rid="bib1.bibx49 bib1.bibx61 bib1.bibx56 bib1.bibx25 bib1.bibx17 bib1.bibx72" id="paren.4"/>.
Such surface temperature anomalies over Eurasia are related to a positive
phase of the Arctic Oscillation, which is forced by interactions between the
stratospheric polar vortex and tropospheric circulation patterns
<xref ref-type="bibr" rid="bib1.bibx31 bib1.bibx38" id="paren.5"/>.</p>
      <p>The overall impact of a tropical eruption on stratospheric ozone chemistry
can be separated into the effect from (i) altered reaction rates due to
change in temperature, (ii) enhanced heterogeneous chemistry from elevated
sulfuric acid aerosol surface area density (SAD), (iii) the temperature and
aerosol changes in modifying the occurrence and types of polar stratospheric
clouds (PSCs), (iv) the composition changes induced by the dynamical
perturbations in the stratosphere, and (v) changes in photolysis rates from
the enhanced aerosol. The temperature change and the reactions on the
heterogeneous aerosol surfaces mainly take place in the aerosol cloud. The
heterogeneous conversion of nitrogen oxides (<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">5</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) into nitric acid
(<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">HNO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) slows down the NO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> cycle of catalytic ozone destruction,
with the effect of increasing ozone concentrations in the middle stratosphere
<xref ref-type="bibr" rid="bib1.bibx66 bib1.bibx59" id="paren.6"/>. In the lower stratosphere, the Cl<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> and HO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula>
cycles are more important with the net chemical effect being ozone loss in
the present-day atmosphere <xref ref-type="bibr" rid="bib1.bibx66 bib1.bibx59 bib1.bibx60" id="paren.7"/>. The
chemical ozone loss from an eruption in the present-day atmosphere is
intensified at high latitudes by a strengthening of the polar vortex, which
reduces temperatures, increasing PSC occurrence. Additionally, the presence
of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> in the polar stratosphere in combination with colder
temperatures facilitates the formation of liquid sulfuric acid ternary
solution particles, which further increase SAD and therefore ozone loss
<xref ref-type="bibr" rid="bib1.bibx13" id="paren.8"/>.</p>
      <p>The net effect of the chemical response further depends on the background
composition of the atmosphere. The slow-down of the NO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> cycle and
heterogeneous reactions intensify the chlorine cycle of ozone destruction,
but chlorine levels have undergone serious changes in the last decades
<xref ref-type="bibr" rid="bib1.bibx58" id="paren.9"/>. In the present-day atmosphere, the elevated halogen
loading in the stratosphere means that the net chemical effect of the
eruption on the global ozone abundance is a reduction
<xref ref-type="bibr" rid="bib1.bibx66 bib1.bibx53 bib1.bibx9" id="paren.10"/>. For low halogen loadings, however,
the chemical effect of the eruption is to increase ozone globally
<xref ref-type="bibr" rid="bib1.bibx66 bib1.bibx3 bib1.bibx9" id="paren.11"/>. Furthermore, increase in the
stratospheric water vapour concentrations associated with the warming of the
tropical tropopause can accelerate the HO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> cycle and reduce ozone even in
the case of low halogen concentrations <xref ref-type="bibr" rid="bib1.bibx36" id="paren.12"/>.</p>
      <p>These effects on stratospheric ozone can broadly be classified into two
distinct groups. The first involves composition-dynamical interactions
associated with the radiative absorption of the volcanic aerosol, which we
refer to as RAD-DYN. The second comprises the net change due to a large
number of heterogeneous chemical reactions on the aerosol surface, which we
refer to as HET-AER. Please note, that the RAD-DYN effect includes also
chemical effects, for instance though changes in the reactions rates or PSC
formation due to the temperature changes. Moreover, HET-AER processes affect
also the radiation transfer through the atmosphere by changes in the chemical
composition.</p>
      <p>From the observations it is not possible to understand which processes are
responsible for the ozone changes and how these changes affect the dynamics.
Using model simulations, the attribution of the ozone changes after the Mt.
Pinatubo eruption has been assessed in several studies
<xref ref-type="bibr" rid="bib1.bibx11 bib1.bibx44 bib1.bibx1 bib1.bibx63 bib1.bibx4" id="paren.13"/>. In
general, these studies conclude that both mechanisms are important, with
regional and seasonal differences.</p>
      <p>In the tropics, total column ozone was observed to reduced after the eruption
of Mt. Pinatubo <xref ref-type="bibr" rid="bib1.bibx47" id="paren.14"/> which was a combined signal of a reduction
in the lower stratosphere and an increase of ozone concentrations above
<xref ref-type="bibr" rid="bib1.bibx33" id="paren.15"/>. The reduction in the lower stratosphere has been
attributed to a mix of the dynamic effect and heterogeneous chemical
reactions <xref ref-type="bibr" rid="bib1.bibx51 bib1.bibx53" id="paren.16"/>. The former reduces ozone by
enhanced up-welling of ozone poor air and the latter via chemical depletion
by active chlorine. Above 18 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> the NO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> deactivation dominates,
increasing ozone with further enhancement in the tropics due to modified
photolysis <xref ref-type="bibr" rid="bib1.bibx44" id="paren.17"/>. A negative feedback between the tropical ozone
changes and aerosol heating has been suggested by <xref ref-type="bibr" rid="bib1.bibx1" id="text.18"/>, with
an reduced heating of up to 25 % in the tropical middle stratosphere.</p>
      <p>Ozone changes in the NH are thought to be primarily caused by the
heterogeneous chemical reaction effects <xref ref-type="bibr" rid="bib1.bibx44 bib1.bibx4" id="paren.19"/>, in
particular at high latitudes
<xref ref-type="bibr" rid="bib1.bibx46 bib1.bibx59 bib1.bibx51 bib1.bibx63 bib1.bibx45" id="paren.20"/>. By
contrast, the increasing ozone observed in the Southern Hemisphere (SH) has
been attributed to dynamical processes induced by the aerosol heating in
combination with the phase of the Brewer–Dobson circulation
<xref ref-type="bibr" rid="bib1.bibx4 bib1.bibx20" id="paren.21"/> or the Quasi-Biennial Oscillation (QBO)
<xref ref-type="bibr" rid="bib1.bibx63 bib1.bibx47" id="paren.22"/>.</p>
      <p>The stratospheric dynamic perturbation after volcanic eruptions originates
mainly from the aerosol heating in the tropical lower stratosphere.
Nevertheless, changes in the ozone concentrations also affect heating rates
and therefore modulate the dynamic response to the eruption
<xref ref-type="bibr" rid="bib1.bibx42" id="paren.23"/>. Using observed ozone anomalies for the Mt. Pinatubo
eruption, <xref ref-type="bibr" rid="bib1.bibx61" id="text.24"/> found a strengthening of the Arctic
Oscillation (AO) in late winter and early spring after the eruption, which is
explained by the cooling effect of the polar stratospheric ozone depletion.
However, by forcing the model with observed ozone anomalies, a separation of
the dynamical and chemical causes of the ozone changes is not possible.
Similar results were found by <xref ref-type="bibr" rid="bib1.bibx55" id="text.25"/> who compared the Mt.
Pinatubo eruption in simulations with and without ozone changes. For
a different climate state (Mt. Tambora, 1815) without anthropogenic chlorine
in the stratosphere, they found a very small influence of the ozone changes
on the dynamical perturbation.</p>
      <p>The purpose of this study is to deepen our understanding of the processes
which drive ozone changes after a strong tropical volcanic eruption and how
these changes modulate atmospheric dynamics in the stratosphere. Moreover, we
assess the influence of the eruption strength on these changes and the role
of different climate setting in moderating the dynamical responses, where the
term climate setting describes a specific atmospheric composition of
greenhouse gases and their effects on the climate system. To the best of our
knowledge these questions have not been addressed before. Here, we use a set
of ensemble sensitivity simulations performed by the
atmosphere–ocean–chemistry–circulation model (AOCCM) SOCOL-MPIOM. To evaluate
the dynamic response, this study focuses mainly on the NH and on the winter
season.</p>
      <p>The paper is structured as follows: Sect. <xref ref-type="sec" rid="Ch1.S2"/> introduces the
coupled AOCCM, the forcing data, and the setup of the experiments. The
results are presented in Sect. <xref ref-type="sec" rid="Ch1.S3"/>, first for the simulated
ozone changes associated with the different processes
(Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>), followed by the dynamical changes
(Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>). Section <xref ref-type="sec" rid="Ch1.S3.SS3"/>
focuses on interactions between the ozone chemistry and the dynamic response
associated with the RAD-DYN effects. Finally, we discuss the results and
present conclusive remarks in Sect. <xref ref-type="sec" rid="Ch1.S4"/>.</p>
</sec>
<sec id="Ch1.S2">
  <title>Model and experiments</title>
<sec id="Ch1.S2.SS1">
  <title>SOCOL-MPIOM</title>
      <p>SOCOL-MPIOM is a coupled atmosphere–ocean–chemistry–climate model
<xref ref-type="bibr" rid="bib1.bibx43" id="paren.26"/>. The atmospheric-chemistry component SOCOL version 3
<xref ref-type="bibr" rid="bib1.bibx54 bib1.bibx62" id="paren.27"/> is based on the physical component MA-ECHAM5
<xref ref-type="bibr" rid="bib1.bibx50 bib1.bibx40" id="paren.28"/>, which is coupled to the chemistry module
MEZON <xref ref-type="bibr" rid="bib1.bibx52 bib1.bibx22" id="paren.29"/>. The chemistry module uses temperature
fields from ECHAM5 and calculates the tendency of 41 gas species, taking into
account 200 gas-phase, 16 heterogeneous, and 35 photolytical reactions.
Heterogeneous reactions are parametrised following <xref ref-type="bibr" rid="bib1.bibx14" id="text.30"/> and
can take place in/on aqueous sulfuric acid aerosols and on three types of
polar stratospheric clouds.</p>
      <p>In the short-wave scheme of SOCOL the solar spectrum is divided into six
spectral intervals. The scheme considers Rayleigh scattering, scattering on
aerosols and clouds, and the absorption of solar irradiance in UV-induced
photolysis reactions, by <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, and 44 other species. In the
near-infrared intervals absorption by water vapour, <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>,
<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, and <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is implemented. Furthermore, a parametrisation
for the absorption of radiation by <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> in the
Lyman-alpha, Schumann–Runge, Hartley and Higgins bands is implemented
following an approach similar to <xref ref-type="bibr" rid="bib1.bibx23" id="text.31"/>. The long-wave scheme
considers frequencies from 10 to 3000 <inline-formula><mml:math display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for the absorption by
water vapour, <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, CFC-11,
CFC-12, CFC-22, aerosols, and clouds. Chemistry–climate interactions can
optionally be disabled in the model, by deactivating the interactive
chemistry module. In this case, 3-D time-dependent ozone data
needs to be applied as forcing.</p>
      <p>The spectral truncation used in this study is T31, which corresponds to
a horizontal resolution of approximately <inline-formula><mml:math display="inline"><mml:mrow><mml:msup><mml:mn>3.75</mml:mn><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:msup><mml:mn>3.75</mml:mn><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula>.
In the vertical, the atmosphere is divided into 39 levels with the highest
level at 0.01 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> (80 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">km</mml:mi></mml:math></inline-formula>). With this vertical resolution the
model is not able to produce a QBO by itself; therefore a QBO nudging is
applied <xref ref-type="bibr" rid="bib1.bibx30" id="paren.32"/>.</p>
      <p>The atmosphere–chemistry model SOCOL is coupled to the ocean model MPIOM
which includes a sea ice module <xref ref-type="bibr" rid="bib1.bibx41 bib1.bibx37" id="paren.33"/>. MPIOM is
used in a nominal resolution of 3<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>, with the poles shifted to
Greenland and Antarctica to avoid numerical singularities at the poles. This
setup allows for a high resolution in the deep water formation region of the
North Atlantic. Both models, MPIOM and SOCOL are coupled by the OASIS3
coupler <xref ref-type="bibr" rid="bib1.bibx12 bib1.bibx69" id="paren.34"/>.</p>
</sec>
<sec id="Ch1.S2.SS2">
  <title>Aerosol forcing data sets</title>
      <p>To simulate the climatic effect of a volcanic eruption in SOCOL-MPIOM, the
model needs information about the optical properties of the aerosols,
including extinction coefficients, single scattering albedo, and the
asymmetry factor for each spectral interval, latitude, vertical level, and
time step. Furthermore, the chemistry module needs the surface area density
(SAD) of the aerosols. In a sensitivity study for different eruption sizes,
these forcings need to be generated in a consistent manner, to allow for
a fair comparison between the eruptions.</p>
      <p>Since nucleation, condensation, coagulation, and sedimentation of the
aerosols change in different ways with the <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> concentration
<xref ref-type="bibr" rid="bib1.bibx68" id="paren.35"/>, a simple linear scaling of observation-based aerosol
data sets by the sulfur mass may lead to an unrealistic forcing data set.
The aerosol coagulation process, for instance, depends on the <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>
concentration, and hence particles tend to be larger as we inject more
<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. The increase in total SAD is hence not proportional to the
increase in <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mass. Conversely, the total stratospheric warming
depends on the aerosol absorption in the infrared and varies more or less
linearly with the <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mass injected <xref ref-type="bibr" rid="bib1.bibx32" id="paren.36"/>. However,
an increase in the sedimentation rates with larger aerosols further modifies the
relationship between the stratospheric warming and the initial sulfur mass
released.</p>
      <p>The aerosol data set used here was therefore calculated offline using the
micro-physical aerosol model AER <xref ref-type="bibr" rid="bib1.bibx70 bib1.bibx71" id="paren.37"/>. AER
is a 2-D model with global domain, resolving the atmosphere from the surface
to approximately 60 km altitude. The vertical resolution is about
1.2 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">km</mml:mi></mml:math></inline-formula> with a horizontal grid spacing of 9.5<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> of
latitude. To simulate the formation of the aerosols, the <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> injection
mass, as well as the timing and latitude/altitude of the injection are used
as inputs for the AER model. Three AER simulations were carried out with 15,
30, and 60 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> injected, the former corresponding
approximately to the <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> detected in the stratosphere shortly after
the Pinatubo eruption <xref ref-type="bibr" rid="bib1.bibx34" id="paren.38"/>. Furthermore, the timing (middle of June)
and the location (5<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–14<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N between 23 and 25 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">km</mml:mi></mml:math></inline-formula>)
are chosen to fit the Pinatubo 1991 eruption. Besides the sulfur mass, the
same set of initial and boundary conditions were applied in all three
simulations, corresponding to the atmospheric state at the time of the
eruption of Mt. Pinatubo in 1991 <xref ref-type="bibr" rid="bib1.bibx26" id="paren.39"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><caption><p>Aerosol data sets used in the simulations for the
15 Tg <bold>(a, b)</bold>, 30 Tg <bold>(c, d)</bold>, and 60 Tg <bold>(e, f)</bold>
<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> aerosol forcing. Surface area densities (SADs) are displayed by
colours; contours denote extinction rates in the visible
(440–690 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">nm</mml:mi></mml:math></inline-formula>) with contours from 0 to 0.05 by an interval of
0.01 <inline-formula><mml:math display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="normal">km</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. The column on the left displays averages for the first
post-eruption winter season (DJF) as a function of pressure and latitude,
while the right column shows Hovmöller diagrams of the monthly mean SAD
forcing at 50 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula>.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="acp-2015-251-f01.pdf"/>

        </fig>

      <p>SAD values and extinction coefficients in the visible are shown in
Fig. <xref ref-type="fig" rid="Ch1.F1"/> for the DJF (December–January–February) season in the first winter after the eruption
on the left and as Hovmoeller diagram for SAD and extinctions at
50 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> on the right. <xref ref-type="bibr" rid="bib1.bibx5" id="text.40"/> found that an injection of
14 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (7 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> of sulfur) produced mid-visible
extinctions much higher than observed in the tropical stratosphere after the
Pinatubo eruption. As shown by <xref ref-type="bibr" rid="bib1.bibx20" id="text.41"/>, the peak burden of sulfur
in the particle phase was around a factor of 2 lower than the peak sulfur
burden in the gas phase, in the range 3.7–6.7 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> of sulfur. The
15 Tg AER simulation shall therefore be regarded as an upper limit for the
perturbation that occurred following Pinatubo. Furthermore, some differences
in the shape of the AER aerosol forcing and observations for Pinatubo exists.
Using satellite based aerosol forcings, the agreement with observations can
be improved for Pinatubo <xref ref-type="bibr" rid="bib1.bibx5" id="paren.42"/>. However, due to the
non-linear relationship between sulfur mass and the aerosol properties
satellite based aerosol records can not be applied in this sensitivity study.
A detailed comparison of satellite based aerosol data sets and the AER method
is given in <xref ref-type="bibr" rid="bib1.bibx5" id="text.43"/>.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <title>Experiments</title>
      <p>A number of ensemble sensitivity experiments were performed. The experiments
differ in the aerosol forcing, the atmospheric composition of different ozone
depleting substances (ODSs) and other greenhouse gases (GHGs), as well as the
physical and chemical processes considered.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><caption><p>Overview of the ensemble experiments used in this study. <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>
mass refers to the aerosol amount assumed in the generation of the volcanic
forcing (compare Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>). Climate setting – PD: 1990s
conditions with high concentrations of ozone depleting substances (ODS). PI:
preindustrial atmosphere with low concentrations of ODS. Volcanic forcing –
SAD: surface area density of the aerosols. OP: optical properties, i.e.
extinction rates for all spectral intervals. For each ensemble, eight simulations
are performed.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="5">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="center"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:colspec colnum="5" colname="col5" align="left"/>
     <oasis:thead>
       <oasis:row>  
         <oasis:entry colname="col1">Ensemble</oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mass</oasis:entry>  
         <oasis:entry colname="col3">Climate setting</oasis:entry>  
         <oasis:entry colname="col4">Volcanic forcing</oasis:entry>  
         <oasis:entry colname="col5">Atm. chemistry</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">(Tg)</oasis:entry>  
         <oasis:entry colname="col3"/>  
         <oasis:entry colname="col4"/>  
         <oasis:entry colname="col5"/>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">PD[15,30,60]</oasis:entry>  
         <oasis:entry colname="col2">15, 30, 60</oasis:entry>  
         <oasis:entry colname="col3">PD</oasis:entry>  
         <oasis:entry colname="col4">SAD and OP</oasis:entry>  
         <oasis:entry colname="col5">interactive</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PI[15,30,60]</oasis:entry>  
         <oasis:entry colname="col2">15, 30, 60</oasis:entry>  
         <oasis:entry colname="col3">PI</oasis:entry>  
         <oasis:entry colname="col4">SAD and OP</oasis:entry>  
         <oasis:entry colname="col5">interactive</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PD[15,30,60]_HET-AER</oasis:entry>  
         <oasis:entry colname="col2">15, 30, 60</oasis:entry>  
         <oasis:entry colname="col3">PD</oasis:entry>  
         <oasis:entry colname="col4">SAD</oasis:entry>  
         <oasis:entry colname="col5">interactive</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PI[15,30,60]_HET-AER</oasis:entry>  
         <oasis:entry colname="col2">15, 30, 60</oasis:entry>  
         <oasis:entry colname="col3">PI</oasis:entry>  
         <oasis:entry colname="col4">SAD</oasis:entry>  
         <oasis:entry colname="col5">interactive</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PD[15,30,60]_RAD-DYN</oasis:entry>  
         <oasis:entry colname="col2">15, 30, 60</oasis:entry>  
         <oasis:entry colname="col3">PD</oasis:entry>  
         <oasis:entry colname="col4">OP</oasis:entry>  
         <oasis:entry colname="col5">interactive</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PI[15,30,60]_RAD-DYN</oasis:entry>  
         <oasis:entry colname="col2">15, 30, 60</oasis:entry>  
         <oasis:entry colname="col3">PI</oasis:entry>  
         <oasis:entry colname="col4">OP</oasis:entry>  
         <oasis:entry colname="col5">interactive</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PD[15,60]_o3</oasis:entry>  
         <oasis:entry colname="col2">15, 60</oasis:entry>  
         <oasis:entry colname="col3">PD</oasis:entry>  
         <oasis:entry colname="col4">–</oasis:entry>  
         <oasis:entry colname="col5">ozone from PD[15, 60]</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PI[15,60]_o3</oasis:entry>  
         <oasis:entry colname="col2">15, 60</oasis:entry>  
         <oasis:entry colname="col3">PI</oasis:entry>  
         <oasis:entry colname="col4">–</oasis:entry>  
         <oasis:entry colname="col5">ozone from PI[15, 60]</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PD[15,60]RAD-DYN_o3</oasis:entry>  
         <oasis:entry colname="col2">15, 60</oasis:entry>  
         <oasis:entry colname="col3">PD</oasis:entry>  
         <oasis:entry colname="col4">–</oasis:entry>  
         <oasis:entry colname="col5">ozone from PD[15, 60]_RAD-DYN</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PI[15,60]RAD-DYN_o3</oasis:entry>  
         <oasis:entry colname="col2">15, 60</oasis:entry>  
         <oasis:entry colname="col3">PI</oasis:entry>  
         <oasis:entry colname="col4">–</oasis:entry>  
         <oasis:entry colname="col5">ozone from PI[15, 60]_RAD-DYN</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PD_CTRL</oasis:entry>  
         <oasis:entry colname="col2">–</oasis:entry>  
         <oasis:entry colname="col3">PD</oasis:entry>  
         <oasis:entry colname="col4">–</oasis:entry>  
         <oasis:entry colname="col5">interactive</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PI_CTRL</oasis:entry>  
         <oasis:entry colname="col2">–</oasis:entry>  
         <oasis:entry colname="col3">PI</oasis:entry>  
         <oasis:entry colname="col4">–</oasis:entry>  
         <oasis:entry colname="col5">interactive</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p>To assess the role of the climate setting on the response, the eruptions
either take place under present-day (early 1990s with high loads of ODS and
GHG in the atmosphere) or preindustrial conditions (early 19th century, low
concentrations of ozone depleting halogens and GHG). The simulations
therefore differ in their atmospheric composition, but also the climate state
is different due to the effect of the GHG on temperature and dynamics. The
initial states for the two periods are based on two transient simulations
described in <xref ref-type="bibr" rid="bib1.bibx43" id="text.44"/>. For the preindustrial climate simulations
the restart files were selected between the years 1812 and 1814. Present-day
initial conditions were extracted between 1988 and 1990. Each ensemble
consists of 8 simulations and the restart files were carefully selected to
cover a wide range of different phases of the Atlantic Meridional Overturning
Circulation and the tropical Pacific (ENSO). The timing of the eruption
(middle of June) is identical for both climate settings.</p>
      <p>For comparison, the simulated response of the climate system after the
volcanic eruption is evaluated against an ensemble of control simulations for
each climate setting. These simulations were initialised using the same set
of initial conditions, but were forced by an aerosol data set representing
the unperturbed background state of the atmosphere.</p>
      <p>To distinguish between the aerosol forcings and the climate setting the
simulations are named PI15, PI30, and PI60 for the eruption sizes of 15, 30,
and 60 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> in the preindustrial conditions,
respectively. The present-day simulations are named PD15, PD30, and PD60,
accordingly. These simulations consider the both radiative and the chemical
aspects of the volcanic forcing (named full aerosol effect in the following)
based on SAD values and optical properties generated by the AER model. Note
that in this study we do not include the effects of the enhanced aerosol in
reducing photolysis, and related composition changes. As explained in Sect.
2.2, the PD15 ensemble simulation represents an upper limit for the effects
from the Mt. Pinatubo eruption in 1991. The PI60 ensemble is comparable to
the Tambora eruption in 1815 <xref ref-type="bibr" rid="bib1.bibx29" id="paren.45"/> although the date of the
eruption and the shape of the aerosol forcings is different
<xref ref-type="bibr" rid="bib1.bibx6" id="paren.46"/>. All aerosol forcing time series were applied as zonal
monthly means between 690 and 3.8 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> and interpolated to the model
levels in SOCOL-MPIOM.</p>
      <p>Furthermore, the effect of stratospheric aerosols on the atmosphere is
separated into radiative-dynamical perturbations (RAD-DYN) and changes
related to heterogeneous chemical reactions on aerosol surfaces (HET-AER). In
the RAD-DYN experiment, only the optical properties of the aerosols was
applied as forcing and the pre-eruption values were used for the SAD. The
HET-AER experiment was forced only with time-varying SAD with the optical
properties representing pre-eruptive conditions. Ensemble experiments with
8 members (Table <xref ref-type="table" rid="Ch1.T1"/>) for both processes were performed for
the three eruption sizes of 15, 30, and 60 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. In the
following these experiments are identified by the suffix _HET-AER and
_RAD-DYN. A summary of the experiments used in this study is given in
Table <xref ref-type="table" rid="Ch1.T1"/>.</p>
      <p>Finally, we extract the simulated ozone changes for the full forcing and
RAD-DYN experiments and apply them as forcing in an additional set of
ensemble simulations. A configuration of SOCOL-MPIOM without interactive
chemistry is used in these experiments <xref ref-type="bibr" rid="bib1.bibx43" id="paren.47"/>. Since ozone
concentrations are not allowed to change, these simulations isolate only the
effect of the ozone changes on the dynamical perturbation. Consequently,
aerosol forcings represent pre-eruptive conditions. Ozone concentrations are
applied as daily mean values on the model grid, to avoid errors due to the
vertical interpolation between pressure levels and model level. These
experiments were performed for the 15 and 60 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> aerosol forcing only.</p>
      <p>The analysis presented mainly focuses on the first winter (DJF) after the
eruption. Results are always expressed in terms of anomalies to the average
of the control ensemble simulations for each climate setting. Significance
estimates are based on a two-tailed Student's <inline-formula><mml:math display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula> test using the 5 %
significance level.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <title>Results</title>
<sec id="Ch1.S3.SS1">
  <title>Ozone changes</title>
<sec id="Ch1.S3.SS1.SSS1">
  <title>Present-day conditions</title>
      <p>The response of the global averaged column ozone (Fig. <xref ref-type="fig" rid="Ch1.F2"/>) reveals
clear differences between the RAD-DYN and the HET-AER effect. In a present-day setup (Fig. <xref ref-type="fig" rid="Ch1.F2"/> top) heterogeneous chemical reactions on the
aerosol surface cause a depletion of global column ozone, which is
significant for more than 2 years. Ozone is continuously reduced for about
9 months after the eruption, independent from the eruption size. However, the
amplitude of the anomaly increases with the eruption size to <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>13, <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>18,
and <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>21 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">DU</mml:mi></mml:math></inline-formula>. The recovery phase lasts about 24 months in all
simulations, again independent of the eruption size. As expected, the spatial
analysis of the HET-AER anomalies shows largest ozone depletion in the high
latitudes of both hemispheres (Fig. <xref ref-type="fig" rid="Ch1.F3"/>a), in particular during
spring and the polar ozone depletion through HET-AER processes increases with
the eruption size (Fig. S1a, d, g in the Supplement).</p>
      <p>Zonally averaged height profiles for the first winter after the eruption
reveal that the aerosol heterogeneous chemical effect also leads to positive
anomalies in the upper stratosphere above 30 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula>
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>a). However, these anomalies are present only in the first
winter after the eruption and are to some extent compensated by negative
anomalies in the lower stratosphere. The positive anomalies in the upper
stratosphere are related to the slow-down of the NO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> cycle of catalytic
ozone destruction, as <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">5</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is converted into <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">HNO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> on the
<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> aerosols. By reducing the NO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> concentrations the reaction
also slows down the deactivation of chlorine, which dominates ozone
destruction in the lower atmosphere and explains the negative anomalies below
30 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula>. Furthermore, the conversion stops, when all <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">5</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is
consumed <xref ref-type="bibr" rid="bib1.bibx66" id="paren.48"/>. In the lower stratosphere <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">5</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is quickly
consumed in the months after the eruption, first in the tropical latitudes,
but about 5 months after the eruptions <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">5</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is reduced by more than
80 % at all latitudes below around 30 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> (not shown). In the NH
and SH polar stratosphere in late winter and spring the heterogeneous
reactions on the aerosol surfaces and on PSCs strongly increase the chlorine
concentrations in the lower stratosphere and explain the pronounced
reductions in ozone.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><caption><p>Monthly mean global mean anomalies of column ozone (DU) for present-day (top) and preindustrial conditions (bottom) for the ensemble simulations
with the full forcing effect (full, solid lines), the ensemble simulations
considering only the heterogeneous aerosol chemical effect of the aerosols
(HET-AER, dotted lines), and the simulations forced only by the
radiative-dynamical aerosol effects (RAD-DYN, dashed lines). The different
eruption sizes are indicated by colours. Lines denote the ensemble mean,
shading the standard deviation of the ensemble.</p></caption>
            <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="acp-2015-251-f02.pdf"/>

          </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><caption><p>Zonal average monthly mean anomalies of total column ozone in
different ensemble simulations: <bold>(a)</bold> anomalies due to the effect of
heterogeneous chemical reactions for the 15 Tg eruption for present-day
conditions. <bold>(b)</bold> Same as <bold>(a)</bold>, but for the
radiative-dynamical effects of the aerosols. <bold>(c)</bold> Same as
<bold>(a)</bold>, but for the full forcing simulations. <bold>(d)</bold> Full forcing
simulations for the 60 Tg aerosol forcing data set. <bold>(e–h)</bold> Similar
to <bold>(a–d)</bold>, but for preindustrial conditions. Stippling in the
simulation panels indicates significant differences to the control (Student's
<inline-formula><mml:math display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula> test <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>p</mml:mi><mml:mo>≤</mml:mo><mml:mn>0.05</mml:mn></mml:mrow></mml:math></inline-formula>). The beginning of the eruption is depicted by the
vertical dashed line.</p></caption>
            <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="acp-2015-251-f03.pdf"/>

          </fig>

      <p>The RAD-DYN effect causes positive global mean column ozone anomalies after
the eruption, which peak about 7 months after the beginning of the eruption
(<inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>5, <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>8, and <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>12 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">DU</mml:mi></mml:math></inline-formula>), and return to background conditions after
about 18 months (Fig. <xref ref-type="fig" rid="Ch1.F2"/>). Similar to the chemical effects, no
clear differences in terms of the duration are found between the three
eruption sizes. The column ozone anomaly time series furthermore reveal some
fluctuations, mainly during the first year. In February–March and
July–August, the positive column ozone anomalies undergo clear reductions.
These variations are related to the present-day polar ozone depletion in the
NH and SH, which is further intensified after the eruption by colder
conditions inside the polar vortices and chlorine activation on the PSCs
(Fig. <xref ref-type="fig" rid="Ch1.F3"/>b). However, the polar ozone depletion in the RAD-DYN
experiment is much weaker than the signal found in the HET-AER ensemble
experiment. For the 15 Tg aerosol forcing the polar ozone depletion is
rather moderate (Fig. <xref ref-type="fig" rid="Ch1.F3"/>b), but the polar ozone depletion
intensifies and lasts longer with increasing forcing strength (Fig. S1e, h).</p>
      <p>Overall, the spatial pattern of ozone anomalies due to the RAD-DYN effect is
more heterogeneous than for the HET-AER effect (Fig. <xref ref-type="fig" rid="Ch1.F3"/>b). Reduced
ozone column abundances are found at tropical latitudes and increasing
concentrations at mid- to high-latitudes. The tropical reduction is related
to pronounced ozone depletion at 30 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula>, which is partly compensated
by positive ozone anomalies above and below (Fig. <xref ref-type="fig" rid="Ch1.F4"/>b). This
equatorial anomaly pattern is very similar for all post-eruption seasons and
remains significant until the end of the first year after the eruption
(Fig. <xref ref-type="fig" rid="Ch1.F3"/>b). The circulation changes in the stratosphere that are
responsible for the ozone anomalies are detected in the residual mean
circulation anomaly <xref ref-type="bibr" rid="bib1.bibx2" id="paren.49"/>. The enhanced vertical transport of
ozone changes the vertical ozone profile and replaces ozone-enhanced air at
30 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> by ozone depleted air from lower levels. Air with enriched
ozone from 30 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> further increases ozone concentrations at
10 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> and above. The upward motion in the tropics is balanced by
descending air masses in the mid-latitudes. Since these air masses originate
from tropical latitudes, they transport ozone enriched air into the lower
stratosphere of the mid-latitudes and create positive ozone anomalies. This
meridional transport is visible in the positive anomalies of column ozone,
which first occur in subtropical latitudes and reach the high latitudes
several months later (Fig. <xref ref-type="fig" rid="Ch1.F3"/>b). A fraction of descending ozone is
recirculated into the lowermost tropical stratosphere and leads to positive
ozone anomalies at 70 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula>. Furthermore, changes in the incoming UV
radiation and photodissociation by the high optical depth of the aerosols may
affect ozone production in the tropics <xref ref-type="bibr" rid="bib1.bibx44" id="paren.50"/>, but this process
is not yet implemented in the model.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><caption><p>Ensemble mean zonal mean ozone mixing ratio anomalies (ppmv) for the
first post eruption DJF season in the present-day ensemble experiment
considering <bold>(a)</bold> the effect of aerosol heterogeneous chemical
reactions <bold>(b)</bold> the radiative-dynamic effect with the 15 Tg aerosol
forcing under present-day conditions. Contour lines in <bold>(a)</bold> denote
the climatological average DJF ozone mixing ratios in the present-day control
ensemble. The streamlines in <bold>(b)</bold> show the residual circulation
anomalies <xref ref-type="bibr" rid="bib1.bibx2" id="paren.51"/>. Stippling indicates significant anomalies
(Student's <inline-formula><mml:math display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula> test <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>p</mml:mi><mml:mo>≤</mml:mo><mml:mn>0.05</mml:mn></mml:mrow></mml:math></inline-formula>).</p></caption>
            <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="acp-2015-251-f04.pdf"/>

          </fig>

      <p>The full aerosol effect displays the combined influence of both processes
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>). In the first 7 months after the eruption,
radiative-dynamical effects dominate the response of ozone with positive
ozone anomalies, which reach maximum values of <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>2, <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>3, and <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>6 DU
between autumn and early winter depending on the 15, 30, and 60 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula>
forcing, respectively (Fig. <xref ref-type="fig" rid="Ch1.F2"/>). In the following months, the
influence of the radiative-dynamical effects weakens, while chemical effects
are still present and column ozone anomalies become negative for about 2
years. The imprint of the intensified polar ozone depletion is clearly
visible in the full forcing experiment. With increasing eruption size the
amplitude of the negative and positive anomalies increases, while the spatial
patterns remain similar (Fig. <xref ref-type="fig" rid="Ch1.F3"/>d and S1f, i). The dynamical
perturbation of the residual circulation by the RAD-DYN effects is also
clearly visible in the full forcing experiments (Fig. S3a, b, c).</p>
</sec>
<sec id="Ch1.S3.SS1.SSS2">
  <title>Preindustrial conditions</title>
      <p>Changing the climatic background conditions from present-day to preindustrial
has a strong impact on the HET-AER effect (Fig. <xref ref-type="fig" rid="Ch1.F2"/> bottom and
Fig. <xref ref-type="fig" rid="Ch1.F3"/>e). Without pronounced amounts of ODS in the stratosphere,
the effect of heterogeneous chemical reactions on the chlorine cycle of ozone
depletion is weak. Instead, the slow-down of the NO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> cycle of ozone
depletion becomes important, explaining slight positive anomalies of column
ozone, for a few months after the eruption. However, with maximum anomalies
between <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>4 and <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>5 DU the response is not very pronounced. The size of
the eruption has no significant effect on the ozone anomalies due to HET-AER
effects (Fig. <xref ref-type="fig" rid="Ch1.F2"/> bottom and S2d, g).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><caption><p>Zonal mean temperature anomalies (K) for the first post eruption
winter (DJF) relative to the average of the present-day or preindustrial
control simulations: <bold>(a)</bold> anomalies due to the effect of
heterogeneous aerosol chemical reactions (HET-AER) for the 15 Tg eruption
under present-day conditions, <bold>(b)</bold> same as <bold>(a)</bold>, but for the
radiative effects of the aerosols, <bold>(c)</bold> same as <bold>(a)</bold>, but
showing the ensemble mean of the full forcing simulations, <bold>(d)</bold> full
forcing simulations for the 60 Tg aerosol forcing data set, and
<bold>(e–h)</bold> similar to <bold>(a)</bold>, but for preindustrial conditions.
Anomalies are calculated relatively to the corresponding control ensemble
mean and the stippling in the simulation panels indicates significant
differences to the control (Student's <inline-formula><mml:math display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula> test <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>p</mml:mi><mml:mo>≤</mml:mo><mml:mn>0.05</mml:mn></mml:mrow></mml:math></inline-formula>). Contours denote
the climatological mean DJF temperatures in the control ensembles.
<bold>(i–l)</bold> Differences between the present-day and preindustrial
temperature anomalies for the different experiments.</p></caption>
            <?xmltex \igopts{width=384.112205pt}?><graphic xlink:href="acp-2015-251-f05.png"/>

          </fig>

      <p>RAD-DYN effects introduce again positive anomalies of column ozone after the
eruption (Figs. <xref ref-type="fig" rid="Ch1.F2"/>, <xref ref-type="fig" rid="Ch1.F3"/>f). In comparison to the present-day ensemble simulations, the anomalies are stronger (<inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>6, <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>14,
<inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>18 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">DU</mml:mi></mml:math></inline-formula>), longer lasting and the variability is lower, which is
explained by the reduced polar ozone depletion in a preindustrial atmosphere.
In fact, the positive anomalies of column ozone cover all latitudes from the
subtropics to polar areas (Fig. <xref ref-type="fig" rid="Ch1.F3"/>f, compare also S2e, h, l).
Consequently, the combined response is dominated by the RAD-DYN effect and
the spatial patterns of the anomaly are very similar (Fig. <xref ref-type="fig" rid="Ch1.F3"/>g).
For larger eruption sizes, the amplitude of the ozone changes due to RAD-DYN
effects increases, while heterogeneous chemical reactions on the aerosols are
only marginally affected by the eruption strength (Fig. <xref ref-type="fig" rid="Ch1.F2"/>).</p>
</sec>
</sec>
<sec id="Ch1.S3.SS2">
  <title>Temperature and dynamics</title>
<sec id="Ch1.S3.SS2.SSS1">
  <title>Present-day conditions</title>
      <p>One motivation of this study is to ask how the ozone changes described in
Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/> modulate the dynamical perturbation of the
stratosphere due to the volcanic eruption.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><caption><p>Similar to Fig. <xref ref-type="fig" rid="Ch1.F5"/>, but for the zonal mean zonal wind
anomalies (<inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>).</p></caption>
            <?xmltex \igopts{width=384.112205pt}?><graphic xlink:href="acp-2015-251-f06.pdf"/>

          </fig>

      <p>Temperature changes associated with an ozone loss due to the HET-AER effect
are small compared to the aerosol direct radiative effect, but significant
temperature reductions are found in the present-day experiments for all three
eruption sizes. For the 15 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> forcing the cooling reach a minimum of
<inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> in the subtropical latitudes of both hemispheres in winter
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>a). These anomalies increase to more than <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>2 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula>
for the 60 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> forcing (not shown). The reduction of the meridional
temperature gradient leads to a significant slow-down of the westerly
circulation in the polar stratosphere during boreal winter
(Fig. <xref ref-type="fig" rid="Ch1.F6"/>a) and a weakening of the polar vortex. As index for the NH
polar vortex intensity, time series of the zonal mean wind component at
60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and 10 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx15 bib1.bibx16" id="paren.52"/>
are shown in Fig. <xref ref-type="fig" rid="Ch1.F7"/>. The weakening of this index due to the
HET-AER effect is mainly a phenomena of the mid to late winter (January,
February). In January the vortex intensity reduces to <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>35</mml:mn><mml:mo>±</mml:mo><mml:mn>15</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> in the PD15_HET-AER experiment in comparison to <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>48</mml:mn><mml:mo>±</mml:mo><mml:mn>11</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> in the CTRL experiment (<inline-formula><mml:math display="inline"><mml:mrow><mml:mn>32</mml:mn><mml:mo>±</mml:mo><mml:mn>18</mml:mn></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>36</mml:mn><mml:mo>±</mml:mo><mml:mn>11</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for the 30 and 60 Tg experiment, respectively. Compare
Fig. <xref ref-type="fig" rid="Ch1.F7"/>). During spring a slight (but not significant) vortex
intensification is found for the stronger forced ensemble simulations. In
March, the mean value of the vortex intensity in CTRL is <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">9</mml:mn><mml:mo>±</mml:mo><mml:mn>18</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, while the vortex in PD15_HET-AER reaches an average
of <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>14</mml:mn><mml:mo>±</mml:mo><mml:mn>15</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math display="inline"><mml:mrow><mml:mn>21</mml:mn><mml:mo>±</mml:mo><mml:mn>19</mml:mn></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>19</mml:mn><mml:mo>±</mml:mo><mml:mn>13</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>
for the 30 and 60 Tg experiment, respectively). This spring intensification
is probably related to the intensified ozone depletion and associated cooling
at polar latitudes. The size of the eruption has no systematic influence on
the vortex changes through the HET-AER effect. The HET-AER effect furthermore
causes slight positive temperature anomalies in the NH polar stratosphere
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>a), which are related to the weakening of the polar vortex.</p>
      <p>The RAD-DYN effects dominate for the temperature perturbations after the
eruption. Significant positive temperature anomalies are found at almost all
altitudes and latitudes, with the exception of the polar areas
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>b). As expected, the temperature anomalies increase with
rising aerosol mass. At 50 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> the maximum temperature anomaly, which
occurs around December, is 9.5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> for the 15 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula> and increases
to 18.2 and 21.7 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> for the 30 and 60 Tg eruptions, respectively. In
the troposphere, the expected cooling due to the reduced incoming short-wave
flux is found at tropical and subtropical latitudes. The stratospheric
warming, however, causes only a weak intensification of the NH polar vortex
(Figs. <xref ref-type="fig" rid="Ch1.F6"/>b, <xref ref-type="fig" rid="Ch1.F7"/>). Significant positive anomalies are found
only for a short period in late winter (February, March) in the case of the
15 Tg aerosol forcing. By contrast the ensemble simulations with the 30 and
60 Tg aerosol forcings reveal a significant intensification of the vortex
during most of the winter (Fig. <xref ref-type="fig" rid="Ch1.F7"/>).</p>
      <p>The amplitude of the temperature change through the HET-AER mechanism is much
weaker than the changes caused by the RAD-DYN effect (Fig. <xref ref-type="fig" rid="Ch1.F5"/>a).
Nevertheless, the temperature reduction causes a significant weakening of the
NH polar vortex, but only a slight increase in the vortex intensity is found
for the RAD-DYN experiment for the 15 Tg aerosol forcing
(Fig. <xref ref-type="fig" rid="Ch1.F7"/>). The difference in the response of the NH polar vortex is
not yet fully understood. It may be related to the different patterns of the
temperature anomaly. The aerosol induced warming covers all latitudes up to
60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N in the lower and middle stratosphere and reaches even polar
latitudes in the upper stratosphere. By contrast, the cooling associated with
the HET-AER effect is limited to the SH and up to 30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N due to the
seasonal cycle of the Brewer–Dobson circulation.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><caption><p>Daily zonal mean zonal wind at 60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N [<inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>]
used as index for the NH polar vortex intensity. Dots at the bottom of each
panel indicate days with significant differences to the control ensemble (<inline-formula><mml:math display="inline"><mml:mrow><mml:mi>p</mml:mi><mml:mo>≤</mml:mo><mml:mn>0.05</mml:mn></mml:mrow></mml:math></inline-formula>). All values are smoothed with an 11 day low pass filter. The start
of the eruption (middle of June) is indicated by the vertical dashed line. The
shading indicates the standard deviation in the control experiments.
Additionally, each panel displays the monthly mean statistics for January
(left) and March (right) with the dots representing the mean value and the
line range corresponding to the standard deviation for each ensemble
experiment.</p></caption>
            <?xmltex \igopts{width=384.112205pt}?><graphic xlink:href="acp-2015-251-f07.pdf"/>

          </fig>

</sec>
<sec id="Ch1.S3.SS2.SSS2">
  <title>Preindustrial conditions</title>
      <p>Under preindustrial conditions the response to an eruption differs in several
aspects. Similar to the ozone anomalies, the HET-AER effect on the
stratospheric temperatures (Fig. <xref ref-type="fig" rid="Ch1.F5"/>e, i) and dynamics is very small
(Figs. <xref ref-type="fig" rid="Ch1.F6"/>e, <xref ref-type="fig" rid="Ch1.F7"/>). No significant anomalies are found, not
even for the strongest forcing scenario although the tendency of a slight NH
polar vortex weakening is apparent, in particular in late winter.</p>
      <p>RAD-DYN effects in a present-day atmosphere slightly differ from the response
under present-day conditions. At 50 hPa the maximum tropical stratospheric
warming is 1.0 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> larger in the present-day atmosphere
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>j) and this differences increases to 2.3 and 1.7 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula>
for the 30 and 60 Tg eruption. The stronger warming under present-day
conditions is not related to the dynamical ozone changes in the RAD-DYN
ensemble experiment, as will be shown below
(Sect. <xref ref-type="sec" rid="Ch1.S3.SS3"/>). A possible explanation could be found
in the different background states. Due to the ozone depletion in the present-day atmosphere, stratospheric ozone concentrations are substantially reduced
in the present-day tropical lower stratosphere. Furthermore, GHGs are higher
for present-day conditions and both differences lead to a colder tropical
stratosphere. With a colder stratosphere and a warmer troposphere the
radiative heating from below is stronger in the present-day atmosphere. For
the combined response in a preindustrial climate setting, no differences to
the RAD-DYN results are found, neither for the 15 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula>
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>g) nor for the stronger forcings.</p>
      <p>In terms of the NH polar vortex, the largest differences between
preindustrial and present-day conditions are found between the two CTRL
experiments (Fig. <xref ref-type="fig" rid="Ch1.F7"/>). In January the vortex is slightly stronger
in the present-day experiment (PD_CTRL: <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>48</mml:mn><mml:mo>±</mml:mo><mml:mn>11</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>;
PI_CTRL: <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>47</mml:mn><mml:mo>±</mml:mo><mml:mn>10</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>), while during March a pronounced and
significant weakening of the vortex is obvious for present day (<inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">9</mml:mn><mml:mo>±</mml:mo><mml:mn>18</mml:mn></mml:mrow></mml:math></inline-formula> vs.
<inline-formula><mml:math display="inline"><mml:mrow><mml:mn>31</mml:mn><mml:mo>±</mml:mo><mml:mn>16</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>). These differences are also related to the
stratospheric temperature differences between preindustrial and present day
caused by different GHGs concentrations. Consequently, pronounced differences
for the RAD-DYN or full forcing effect would be found between preindustrial
and present day, when the vortex response is expressed in terms of anomalies
to the corresponding CTRL.</p>
</sec>
</sec>
<sec id="Ch1.S3.SS3">
  <title>Effects of the coupling between ozone and stratospheric dynamics on the stratosphere</title>
      <p>The simulated ozone changes due to the RAD-DYN effect or in the full forcing
response could amplify or weaken the dynamical perturbation of the
stratosphere. However, from the results described above, possible feedbacks
between the ozone chemistry and the dynamics are difficult to extract. Two
additional sensitivity ensemble experiments were therefore performed, driven
only by the simulated ensemble mean ozone changes obtained from the RAD-DYN
and full forcing experiments (shown for instance in Figs. <xref ref-type="fig" rid="Ch1.F2"/> and
<xref ref-type="fig" rid="Ch1.F3"/>).</p>
      <p>Zonal mean temperature anomalies (Fig. <xref ref-type="fig" rid="Ch1.F8"/>) reveal an amplification
of the RAD-DYN heating in the lower tropical stratosphere by the ozone
chemistry. At these levels, ozone anomalies up to 0.2 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">ppmv</mml:mi></mml:math></inline-formula>
(25 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">%</mml:mi></mml:math></inline-formula>) are found in the PD15_RAD-DYN ensemble mean, resulting in
temperature anomalies of about <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>1.2</mml:mn><mml:mo>±</mml:mo><mml:mn>0.3</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> (80 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula>) during
the first winter season after the eruption (Fig. <xref ref-type="fig" rid="Ch1.F8"/>a). Ozone
anomalies and temperature anomalies increase with eruption size and reach
0.4 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">ppmv</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>2.9</mml:mn><mml:mo>±</mml:mo><mml:mn>0.5</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> for the 60 Tg eruption the
present-day experiments (Fig. <xref ref-type="fig" rid="Ch1.F8"/>c). For the ozone changes extracted
from the full forcing experiment, the impact on tropical stratospheric
temperatures is always weaker, due to the ozone depleting effect of
heterogeneous chemical reactions (Fig. <xref ref-type="fig" rid="Ch1.F8"/>b, d). Under preindustrial
conditions, the response is slightly stronger, but the differences are not
significant (Fig. <xref ref-type="fig" rid="Ch1.F8"/>e, f, g, h).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8" specific-use="star"><caption><p>Similar to Fig. <xref ref-type="fig" rid="Ch1.F5"/> but showing DJF zonal mean temperature
anomalies (K) in the ozone sensitivity ensemble experiment. (top) Present day
ensemble experiments forced by ozone changes from PD15_RAD-DYN <bold>(a)</bold>,
PD15 <bold>(b)</bold>, PD60_RAD-DYN <bold>(c)</bold>, and PD60 <bold>(d)</bold>.
(bottom) Same forcings but for the preindustrial experiments. Note the
different colour scaling in comparison to Fig. <xref ref-type="fig" rid="Ch1.F5"/>.</p></caption>
          <?xmltex \igopts{width=384.112205pt}?><graphic xlink:href="acp-2015-251-f08.pdf"/>

        </fig>

      <p>The combined influence of HET-AER and RAD-DYN mechanisms is again visible in
the full forcing experiment. The stratospheric warming is slightly reduced by
heterogeneous chemical reactions (8.7 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> in PD15) and the dynamical
changes are weaker in comparison to the RAD-DYN experiment
(Fig. <xref ref-type="fig" rid="Ch1.F6"/>c). In particular the NH polar vortex weakening in January
and the strengthening in March caused by the HET-AER effect is clearly
visible in the <inline-formula><mml:math display="inline"><mml:mover accent="true"><mml:mi mathvariant="normal">u</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover></mml:math></inline-formula>60 index (Fig. <xref ref-type="fig" rid="Ch1.F7"/>).</p>
      <p>RAD-DYN ozone changes in the tropics furthermore produce a cooling above
30 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> with temperature anomalies from <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>2 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> (15 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula>)
to <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>4 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> (60 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">Tg</mml:mi></mml:math></inline-formula>). Ozone changes in this region therefore
weaken the warming effect of the aerosols. Heterogeneous chemical reactions
have no effect on temperatures in this region and ozone changes from the
RAD-DYN and the full forcing ensemble simulations lead to very similar
temperature patterns. Temperature anomalies in a preindustrial atmosphere do
not significantly differ from the results obtained under present day
conditions. Note, that the cold anomaly in the upper stratosphere and
mesosphere (present in all panels of Fig. <xref ref-type="fig" rid="Ch1.F8"/>) can not be attributed
to volcanic induced ozone anomalies but is related to the missing diurnal
cycle of ozone variations in SOCOL-MPIOM without interactive chemistry
<xref ref-type="bibr" rid="bib1.bibx43" id="paren.53"/>.</p>
      <p>Furthermore, positive temperature anomalies are found in the NH polar
stratosphere, though not significant except for one experiment (ozone changes
from PD15_RAD-DYN). Since ozone anomalies in the NH polar stratosphere are
very weak during the first winter after an eruption, these warm anomalies are
probably not related to the ozone chemistry, but to dynamical changes.</p>
      <p>The effect of the ozone perturbations on the NH polar vortex is in general
small (Fig. <xref ref-type="fig" rid="Ch1.F7"/>) and not always consistent. Nevertheless, all
experiments under present-day conditions reveal a slight weakening of the
vortex, which is significant for a few days in mid-winter, and a slight (non
significant) intensification in late winter. The size of the anomalies is
roughly comparable to the changes related to the HET-AER effect. The response
of the vortex to the ozone changes from the RAD-AER and full forcing
experiment is weaker and not significant when ensemble simulations under
preindustrial conditions are considered.</p>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <title>Discussion and conclusions</title>
      <p>This study
addresses the role of ozone changes for the dynamical perturbations of the
stratosphere after strong tropical volcanic eruptions. Thereby, the
underlying mechanisms and the influence of the climate setting and the
eruption strengths are considered. The results are based on a number of
ensemble sensitivity simulations with the AOCCM SOCOL-MPIOM, which allows us
to separate the effect of heterogeneous chemical reactions from the warming
effect of the aerosols for preindustrial and present-day conditions as well
as three different eruption intensities.</p>
      <p>In agreement with earlier studies we find that both processes, heterogeneous
chemical reactions on the aerosol surface and the warming effect of the
aerosols are important for the ozone changes after the eruption in an
atmosphere with enhanced concentrations of ODS
<xref ref-type="bibr" rid="bib1.bibx44 bib1.bibx1" id="paren.54"/>. A comparable case-study for the 1991 Mt.
Pinatubo was performed by <xref ref-type="bibr" rid="bib1.bibx4" id="text.55"/>, with a similar separation
between radiative-dynamical and heterogeneous chemical effects on the
aerosols. They identified a combination of HET-AER and RAD-DYN processes to
be responsible for the ozone anomalies in the SH. In particular they found
similar anomalies in the residual mean circulation being responsible for
reduced ozone in the tropics and enhanced ozone concentrations at
mid-latitudes (compare Fig. <xref ref-type="fig" rid="Ch1.F4"/>b and their Fig. 7). This response,
however, is limited to the early phase of the eruptions and in combination
with the phase of the Brewer–Dobson circulation the anomaly-pattern is found
only in the SH. In boreal winter, when tropical stratospheric temperature
anomalies are at maximum in our experiments, our findings suggest a similar
response of the residual mean circulation in the NH with positive column
ozone anomalies at mid-latitudes. <xref ref-type="bibr" rid="bib1.bibx4" id="text.56"/> did not simulate
positive column ozone anomalies in the NH related to radiative-dynamical
changes (compare their Fig. 6) and concluded that NH ozone anomalies are
mainly affected by HET-AER effects. This difference in the response is not
yet understood, but may be related to differences in the aerosol forcings.
Understanding the response to the RAD-DYN mechanism is of particular
importance for volcanic eruptions under preindustrial conditions with low
load of ozone depleting halogens, where chemical effects become weak and the
response is dominated by radiative-dynamical effects.</p>
      <p>The dynamical perturbation of the stratosphere is dominated by the RAD-DYN
effect of the aerosols. During winter time, the warming in the tropical
stratosphere increases the meridional temperature gradient towards the poles
and strengthens the westerly circulation in the polar stratosphere. Ozone
changes, related to heterogeneous chemical reactions on aerosols under
present-day conditions weaken the warming in the tropical stratosphere and
the NH polar vortex. By contrast, ozone changes related to the RAD-DYN
mechanism amplify the warming in the subtropical and mid-latitude lower
stratosphere, but weaken the temperature response in the middle stratosphere.
The latter causes a slight weakening of the polar vortex. In agreement with
<xref ref-type="bibr" rid="bib1.bibx61" id="text.57"/> and <xref ref-type="bibr" rid="bib1.bibx55" id="text.58"/> we found an intensification
of the NH polar vortex in late winter due to ozone changes after strong
volcanic eruptions in a present-day atmosphere. Our results show that both,
HET-AER and RAD-DYN effects contribute to this intensification.</p>
      <p>The atmospheric composition influences the response of the ozone chemistry
and the dynamical response to the volcanic aerosols in a significant way. As
already shown by <xref ref-type="bibr" rid="bib1.bibx66" id="text.59"/> heterogeneous chemical reactions on the
aerosol surface cause pronounced global ozone depletion when stratospheric
loads of ozone depleting halogens are high, but has only a weak positive
effect in a preindustrial atmosphere. Furthermore, ozone depletion scales
with the amplitude of eruptions under present-day conditions, but for a
preindustrial atmosphere the response is independent from the eruption size
<xref ref-type="bibr" rid="bib1.bibx66" id="paren.60"/>. With the projected reduction of ODS
<xref ref-type="bibr" rid="bib1.bibx7 bib1.bibx24 bib1.bibx8" id="paren.61"/> the effect of heterogeneous chemical
reactions can be expected to become less important for future eruptions.
However, differences in the background state affect the results of this study
as well. In recent decades, the stratosphere has undergone a pronounced
cooling trend <xref ref-type="bibr" rid="bib1.bibx65" id="paren.62"><named-content content-type="pre">e.g.</named-content></xref>, related to the ozone changes and
the increasing levels of GHG <xref ref-type="bibr" rid="bib1.bibx57" id="paren.63"/>. This cooling also affects the
meridional temperature profiles in the stratosphere and the dynamics. In this
study, significant differences in the vortex behaviour exist between the
control simulations for preindustrial and present day, and these differences
can be larger than the differences between the simulations perturbed by the
volcanic eruption.</p>
      <p>A direct comparison of our results to observations is difficult given the
highly idealised character of our experiments. Nevertheless, one experiment,
the 15 Tg experiment for the full aerosol effects under present-day
conditions, can be considered similar to the perturbation from Pinatubo in
1991. Globally, the combined aerosol effect for the 15 Tg aerosol forcing
results in an ozone loss of <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>10.4</mml:mn><mml:mo>±</mml:mo><mml:mn>3.7</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">DU</mml:mi></mml:math></inline-formula> 21 months after the
start of the eruption. This agrees reasonably well with observations for
Pinatubo <xref ref-type="bibr" rid="bib1.bibx10" id="paren.64"/>, where a reduction of <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>13.9 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">DU</mml:mi></mml:math></inline-formula> was
observed peaking in May 1993 (22 months after the eruption). Furthermore, the
pattern of column ozone anomalies in <xref ref-type="bibr" rid="bib1.bibx10" id="text.65"/> is similar to the
pattern found in the PD15 ensemble mean (Fig. <xref ref-type="fig" rid="Ch1.F3"/>). After the
eruption, negative anomalies are found in the tropics and positive anomalies
in the sub-tropics and mid latitudes. The magnitude of both is stronger in
SOCOL-MPIOM than in observations. In particular, the positive column ozone
anomaly in the NH mid-latitudes is weaker in the <xref ref-type="bibr" rid="bib1.bibx10" id="text.66"/> data
set. This may be related to the QBO effect <xref ref-type="bibr" rid="bib1.bibx63 bib1.bibx47" id="paren.67"/> or
the Brewer–Dobson circulation <xref ref-type="bibr" rid="bib1.bibx4" id="paren.68"/>, which modulated the ozone
anomalies after Pinatubo. The modulating effect of the QBO, however, has been
removed by the comparison to an ensemble of control simulations nudged by the
same QBO reconstruction. Overestimated ozone anomalies in the PD15 ensemble
may further be related to the too strong warming simulated in the tropical
stratosphere by SOCOL-MPIOM. The remaining anomalies, i.e. the polar ozone
depletion and the global reduction of columns ozone about 1 year after the
eruptions agrees reasonable well with the simulated anomalies. For the
vertical pattern of ozone changes <xref ref-type="bibr" rid="bib1.bibx35" id="paren.69"><named-content content-type="pre">e.g.</named-content></xref> the agreement
between model results and observations is also reasonable, with the exception
of stronger anomalies in the model, in particular in the tropics.</p>
      <p>A caveat of this study is the overestimated warming in the tropical
stratosphere, which may lead to an overestimation of the dynamical response
and the resulting ozone changes. This needs to be considered when
interpreting the results of the RAD-DYN and full forcing ensemble results. An
overestimation of the lower stratospheric warming after volcanic eruptions is
a feature common to many models <xref ref-type="bibr" rid="bib1.bibx21" id="paren.70"><named-content content-type="pre">e.g.</named-content></xref>. The maximum
warming after the Pinatubo eruption in a multi-model ensemble average of
13 CMIP5 models <xref ref-type="bibr" rid="bib1.bibx21" id="paren.71"><named-content content-type="pre">model selection as in</named-content></xref> is <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>3.8</mml:mn><mml:mo>±</mml:mo><mml:mn>2.9</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> for the temperature anomaly at 50 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula>, while
reanalysis products and observations suggest temperature anomalies between
2.5 and 3 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx39 bib1.bibx19" id="paren.72"/>. However, the phase of the
QBO and other dynamical processes are suggested to reduce the stratospheric
warming after Pinatubo <xref ref-type="bibr" rid="bib1.bibx21 bib1.bibx28" id="paren.73"/>. SOCOL-MPIOM
simulates a warming of <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>8.7</mml:mn><mml:mo>±</mml:mo><mml:mn>1.2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> in the PD15 ensemble. Our
results show that the overestimated warming is to some extent related to the
ozone changes, which amplify the warming by about 0.9 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula> (15 Tg
forcing at 50 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula>). The aerosol forcing applied in this study also
contributes to the overestimated warming. We use a 2-D global aerosol forcing
produced by an aerosol micro-physical model, which allows us to generate
physical consistent forcing for different eruption intensities. This
model-generated forcing differs from satellite based observations for
Pinatubo in several aspects <xref ref-type="bibr" rid="bib1.bibx5" id="paren.74"><named-content content-type="pre">as described by</named-content></xref>. For
comparison, we also perform eight simulations forced by realistic satellite
based aerosol concentrations for the Mt. Pinatubo eruption
<xref ref-type="bibr" rid="bib1.bibx5" id="paren.75"><named-content content-type="pre">SAGE_4<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">λ</mml:mi></mml:math></inline-formula> in</named-content></xref>. In these simulations (not
shown) the stratospheric warming is still overestimated (maximum temperature
anomalies: <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>6.0</mml:mn><mml:mo>±</mml:mo><mml:mn>1.0</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">K</mml:mi></mml:math></inline-formula>), but the agreement to CMIP5 is better, in
particular when the temperature effect of the ozone changes is considered.</p>
      <p>In summary, we show that ozone is affected globally by a volcanic eruption
for several years. Both effects, the radiative dynamical perturbation by the
volcanic aerosols as well as the heterogeneous chemical reaction on the aerosols
are important for the response of the ozone chemistry. The climate setting,
in particular the atmospheric concentrations of ODS, has the strongest
effects on the heterogeneous chemical effect on aerosol surfaces with
pronounced global ozone depletion for present-day ODS concentrations (peak
reductions of <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>13, <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>18, and <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>21 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">DU</mml:mi></mml:math></inline-formula> for the 15, 30, and 60 Tg
eruptions, respectively) and slight ozone increase for preindustrial ODS
concentrations (between 4 and 5 DU for all eruptions). Radiative dynamical
ozone changes are positive for preindustrial and present-day conditions, but
for present day the response is weakened by amplified polar ozone depletion
(<inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>5, <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>8, <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>12 DU peak column ozone anomalies for present day and <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>6,
<inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>14, <inline-formula><mml:math display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>18 DU for preindustrial). The full effect of the volcanic aerosol,
therefore, clearly differs between preindustrial and present day, with long
lasting ozone depletion in a present-day atmosphere and positive ozone
anomalies for preindustrial conditions. The response of stratospheric
temperature and dynamics is dominated by the radiative heating effect of the
aerosols. A small influence of the climate setting on the heating of the
lower tropical stratosphere was found, with larger temperature anomalies for
the present-day experiments. Dynamical radiative ozone changes further
amplify the stratospheric temperature anomalies in the lower tropical
stratosphere (and cause a cooling in higher levels). Ozone changes due to
heterogeneous chemical reactions on the aerosols are responsible for a slight
cooling of the tropical stratosphere. In winter and early spring after the
eruption, the NH polar vortex is intensified, due to the radiative warming in
the tropical stratosphere. Ozone changes, either due to radiative-dynamical
effects or heterogeneous reaction on the aerosol surface, induce a slight
weakening of the vortex in mid-winter. In late winter they cause a slight
strengthening of the westerly circulation in the NH polar stratosphere.</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-15-11461-2015-supplement" xlink:title="pdf">doi:10.5194/acp-15-11461-2015-supplement</inline-supplementary-material>.</bold></p></supplementary-material>
        </app-group><ack><title>Acknowledgements</title><p>We would like to thank the two anonymous reviewers for their constructive
comments. This work has been supported by the Swiss National Science
Foundation under grant CRSII2-147659 (FUPSOL II) and profited from
discussions during the PAGES/FUPSOL Workshop in 2014. <?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>
Edited by: K. Tsigaridis</p></ack><ref-list>
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