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<article xmlns:xlink="http://www.w3.org/1999/xlink" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:oasis="http://docs.oasis-open.org/ns/oasis-exchange/table" dtd-version="3.0"><?xmltex \makeatother\@nolinetrue\makeatletter?>
  <front>
    <journal-meta>
<journal-id journal-id-type="publisher">ACP</journal-id>
<journal-title-group>
<journal-title>Atmospheric Chemistry and Physics</journal-title>
<abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title>
<abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys.</abbrev-journal-title>
</journal-title-group>
<issn pub-type="epub">1680-7324</issn>
<publisher><publisher-name>Copernicus Publications</publisher-name>
<publisher-loc>Göttingen, Germany</publisher-loc>
</publisher>
</journal-meta>

    <article-meta>
      <article-id pub-id-type="doi">10.5194/acp-16-15581-2016</article-id><title-group><article-title>Projection of North Atlantic Oscillation and its effect on <?xmltex \hack{\newline}?>tracer transport</article-title>
      </title-group><?xmltex \runningtitle{NAO projection and tracer transport}?><?xmltex \runningauthor{S. Bacer et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Bacer</surname><given-names>Sara</given-names></name>
          <email>sara.bacer@mpic.de</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Christoudias</surname><given-names>Theodoros</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-9050-3880</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Pozzer</surname><given-names>Andrea</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-2440-6104</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Atmospheric Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Computation-based Science and Technology Research Center, The Cyprus Institute, Nicosia, Cyprus</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Sara Bacer (sara.bacer@mpic.de)</corresp></author-notes><pub-date><day>16</day><month>December</month><year>2016</year></pub-date>
      
      <volume>16</volume>
      <issue>24</issue>
      <fpage>15581</fpage><lpage>15592</lpage>
      <history>
        <date date-type="received"><day>11</day><month>May</month><year>2016</year></date>
           <date date-type="rev-request"><day>20</day><month>May</month><year>2016</year></date>
           <date date-type="rev-recd"><day>23</day><month>November</month><year>2016</year></date>
           <date date-type="accepted"><day>25</day><month>November</month><year>2016</year></date>
      </history>
      <permissions>
<license license-type="open-access">
<license-p>This work is licensed under a Creative Commons Attribution 3.0 Unported License. To view a copy of this license, visit <ext-link ext-link-type="uri" xlink:href="http://creativecommons.org/licenses/by/3.0/">http://creativecommons.org/licenses/by/3.0/</ext-link></license-p>
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</permissions><self-uri xlink:href="https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016.html">This article is available from https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016.html</self-uri>
<self-uri xlink:href="https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016.pdf</self-uri>


      <abstract>
    <p>The North Atlantic Oscillation (NAO) plays an important role in the climate
variability of the Northern Hemisphere, with significant consequences on
long-range pollutant transport. We investigate the evolution of pollutant
transport in the 21st century influenced by the NAO under a global climate
change scenario. We use a free-running simulation performed by the
ECHAM/MESSy Atmospheric Chemistry (EMAC) model coupled with the ocean general
circulation model MPIOM, covering the period from 1950 until 2100. Similarly
to other works, the model shows a future northeastward shift of the NAO
centres of action and a weak positive trend of the NAO index (over
150 years). Moreover, we find that NAO trends (computed over periods shorter
than 30 years) will continue to oscillate between positive and negative
values in the future. To investigate the NAO effects on transport we consider
carbon monoxide tracers with exponential decay and constant interannual
emissions. We find that at the end of the century, the south-western
Mediterranean and northern Africa will, during positive NAO phases, see
higher pollutant concentrations with respect to the past, while a wider part
of northern Europe will, during positive NAO phases, see lower pollutant
concentrations. Such results are confirmed by the changes observed in the
future for tracer concentration and vertically integrated tracer transport,
differentiating the cases of “high NAO” and “low NAO” events.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

      <?xmltex \hack{\newpage}?>
<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p>The North Atlantic Oscillation (NAO) is the most prominent recurrent pattern
of atmospheric variability over middle and high latitudes in the Northern
Hemisphere (NH). It is a swing between two pressure systems, the Azores High
and Icelandic Low, which redistribute atmospheric masses between the Arctic
and the subtropical Atlantic, influencing weather conditions <xref ref-type="bibr" rid="bib1.bibx51" id="paren.1"/>.
When the Icelandic Low and Azores High are relatively stronger, the pressure
difference is higher than average (positive NAO phase) and the north–south
pressure gradient produces surface westerlies stronger than average across
the middle latitudes of the Atlantic towards northern Europe. On the other
hand, when the low and high surface pressures are relatively weaker (negative
NAO phase), the flow has a reduced zonal component. These meridional
oscillations produce large changes in the mean wind speed and direction, heat
and moisture transport, surface temperature and intensity of precipitation,
especially during boreal winter <xref ref-type="bibr" rid="bib1.bibx20" id="paren.2"><named-content content-type="post">and references
therein</named-content></xref>. Several studies
<xref ref-type="bibr" rid="bib1.bibx18 bib1.bibx50 bib1.bibx20" id="paren.3"/> have associated the westerly flow
during positive NAO with warm and moist maritime air and enhanced
precipitation over north-western Europe, and colder and drier conditions over
the Mediterranean.</p>
      <p>As the NAO exerts a strong influence on the boreal winter weather, it can
also affect the transport of gas pollutants on a hemispheric scale. <xref ref-type="bibr" rid="bib1.bibx28" id="normal.4"/>
examined the transatlantic transport of anthropogenic ozone and the NAO
impacts on the surface ozone in North America and Europe; they found that
there are higher northern American ozone concentrations at Mace Head,
Ireland, during positive NAO, when westerly winds across the North Atlantic are
stronger. <xref ref-type="bibr" rid="bib1.bibx3" id="normal.5"/> also analysed the relationship between the NAO
phases and the tropospheric ozone transport across the North Atlantic and
discovered that rises of ozone over western Europe are strongly correlated
with positive NAO. <xref ref-type="bibr" rid="bib1.bibx7" id="normal.6"/> studied the relationship between the NAO
and transport towards the Arctic and found that concentrations of surface
carbon monoxide, originating from both Europe and North America, increase in
the Arctic during the NAO positive phases. <xref ref-type="bibr" rid="bib1.bibx2" id="normal.7"/> studied the
transport of regionally tagged, idealized tracers in relation to the NAO and
found that, during high positive NAO phases, the trace gases emitted from
North America are transported relatively far to north-eastern Europe,
while the trace gases emitted over Europe are transported mostly over Africa
and the Arctic Circle. <xref ref-type="bibr" rid="bib1.bibx34" id="normal.8"/> showed with both station
measurements and coupled atmosphere–chemistry model simulations that the NAO
affects surface ozone concentrations during all seasons, except for in autumn.
The sensitivity studies by <xref ref-type="bibr" rid="bib1.bibx48" id="normal.9"/> regarding the free tropospheric
carbon monoxide concentrations to different atmospheric weather conditions
confirmed the NAO control of pollutant distribution and transport over the
Nordic countries.</p>
      <p>A number of studies have focused on the impacts of the NAO on aerosol
concentrations. <xref ref-type="bibr" rid="bib1.bibx31" id="normal.10"/> analysed the role of the NAO in controlling the
desert-dust transport into the Atlantic and Mediterranean and suggested that
the NAO likely influences the distribution of anthropogenic aerosols.
<xref ref-type="bibr" rid="bib1.bibx21" id="normal.11"/> investigated the NAO influence on European aerosol
concentrations through local atmospheric processes (e.g. precipitation,
wind, cloudiness) and found that positive NAO promotes higher ground-level
aerosol concentrations in southern regions of the Mediterranean during
winter. <xref ref-type="bibr" rid="bib1.bibx35" id="normal.12"/> proved the influence of the NAO extreme events
during the 1990s on the variability of particulate matter concentrations over
Europe, and suggested the usage of the NAO index as a proxy for health impacts
of pollution. The aforementioned studies suggest that future NAO phases will
be important when projecting the northern American and European pollutant
transport over Europe and the Arctic.</p>
      <p>The NAO is an intrinsic mode of atmospheric variability but there is mounting
evidence in the literature that it is unlikely that only stochastic
atmospheric processes are the cause of NAO changes. There are a few candidate
mechanisms to interpret low-frequency variations such as the North Atlantic
<xref ref-type="bibr" rid="bib1.bibx40" id="paren.13"/> and tropical <xref ref-type="bibr" rid="bib1.bibx16" id="paren.14"/> sea-surface temperature (SST),
the sea-ice variations in the North Atlantic Ocean <xref ref-type="bibr" rid="bib1.bibx30" id="paren.15"/> and the
stratospheric circulation <xref ref-type="bibr" rid="bib1.bibx1" id="paren.16"/>. Recently, <xref ref-type="bibr" rid="bib1.bibx52" id="normal.17"/> have
ascribed the NAO variability on interannual–decadal timescales to the
latitudinal variations of the North Atlantic jet and storm track, and the NAO
variability on longer timescales to their speed and strength changes. In
order to explain the upward trend observed from the 1960s until 1990s, some
external forcings have been proposed as responsible. They include the
increase of greenhouse gases <xref ref-type="bibr" rid="bib1.bibx25" id="paren.18"/>, warmer tropical SST
<xref ref-type="bibr" rid="bib1.bibx16" id="paren.19"/> and the strengthened stratospheric vortex <xref ref-type="bibr" rid="bib1.bibx1" id="paren.20"/>.
However, there is still no consensus and <xref ref-type="bibr" rid="bib1.bibx33" id="normal.21"/> asserted that recent
variations can not be explained, even when combining the anthropogenic
forcing and internal variability. Thus, a conclusive understanding of past
NAO variability has still to be reached, and the future NAO evolution
continues to be an open research topic.</p>
      <p>Earth system model simulations with increasing greenhouse-gas (GHG)
concentrations can provide projections of the NAO and future trends. Most
models have projected a weak positive NAO trend under a global warming
climate change scenario. <xref ref-type="bibr" rid="bib1.bibx15" id="normal.22"/> found this when considering the
mean of 37 CMIP5 models' merged historical and RCP 4.5 simulations for each
season, and <xref ref-type="bibr" rid="bib1.bibx47" id="normal.23"/> obtained similar results to 14 models out of
18 studied. However, some studies found the NAO index in a future scenario
only weakly sensitive to the GHG increment, with no significant trends
<xref ref-type="bibr" rid="bib1.bibx12 bib1.bibx5 bib1.bibx39 bib1.bibx10" id="paren.24"/>, or even decreasing trends
<xref ref-type="bibr" rid="bib1.bibx33" id="paren.25"/>. More recently, <xref ref-type="bibr" rid="bib1.bibx36" id="normal.26"/> analysed the impacts due to
the aerosol reduction (after air pollution mitigation strategies) and GHG
increment on the winter North Atlantic atmospheric circulation and obtained a
stronger positive NAO mean state by 2030. The dependency of the results on
the model used is still unclear <xref ref-type="bibr" rid="bib1.bibx14 bib1.bibx47" id="paren.27"/>. Other research
questions are still open, regarding which climate processes govern the NAO
variability, how the phenomenon varies in time, and what is the potential for
the NAO predictability <xref ref-type="bibr" rid="bib1.bibx50 bib1.bibx19 bib1.bibx52" id="paren.28"/>.</p>
      <p>The distribution and development of gases and aerosols are controlled by
atmospheric chemistry and physics, including the transport of air masses
integrated on a continental scale. A large number of studies have addressed
the NAO influence on tracer transport and the future trends of the NAO as
disparate topics. However, there are no studies on the influence of the NAO
on tracer and pollutant transport under a future scenario using an integrated
modelling approach and with full atmospheric chemistry to account for all
potential feedbacks.</p>
      <p>The aim of this paper is to study the influence on the pollutant transport
due to the NAO in the span of the 21st century using a full Earth system
model. We analyse a simulation performed by a coupled
atmosphere–chemistry–ocean general circulation model in order to
(i) investigate the NAO signal and trend in the future and (ii) study the NAO
influence on the pollutant transport in the past and in the future over the
North Atlantic sector. For the analysis, we focus on the carbon monoxide
(<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula>) pollutant, which is directly emitted by combustion sources and
has a lifetime of 1–3 months in the atmosphere; thus, it has a sufficiently
long atmospheric residence lifetime relative to the timescales of transport.</p>
      <p>The paper is structured as follows: Sect. <xref ref-type="sec" rid="Ch1.S2"/> briefly
describes the model used and the simulation set-up;
Sect. <xref ref-type="sec" rid="Ch1.S3"/> presents the NAO trends of the future projection;
Sect. <xref ref-type="sec" rid="Ch1.S4"/> analyses the NAO influence on and the changes in tracer transport.
Conclusions and outlook are given in Sect. <xref ref-type="sec" rid="Ch1.S5"/>.</p>
</sec>
<sec id="Ch1.S2">
  <title>Methodology</title>
      <p>Increasingly, the dynamics and chemistry of the atmosphere are being
studied and modelled in unison in global models.
Starting with the fifth round of the Coupled Model Intercomparison
Project Phase 5 (CMIP5), some of the Earth system models (ESMs) that participated
with interactive oceans included calculations of interactive chemistry.
It was also a main recommendation of the <xref ref-type="bibr" rid="bib1.bibx46" id="normal.29"/>,
that chemistry–climate models (CCMs) should continue to evolve towards
more comprehensive, self-consistent stratosphere–troposphere CCMs. These
developments allow for the inclusion of a better representation of
stratosphere–troposphere, chemistry–climate and atmosphere–ocean couplings in
CCMs and ESMs used for more robust predictions of
climate changes and mutual influences and feedbacks on emitted pollutants <xref ref-type="bibr" rid="bib1.bibx8" id="paren.30"/>.
The ECHAM/MESSy Atmospheric Chemistry (EMAC) model was one of
the first community models to introduce all these processes <xref ref-type="bibr" rid="bib1.bibx22" id="paren.31"/>.</p>
      <p>In this work we analyse a long chemistry climatic simulation performed by the
EMAC climate model under the Earth System Chemistry integrated Modelling
(ESCiMo) initiative
<xref ref-type="bibr" rid="bib1.bibx24" id="paren.32"/>. The EMAC model is a numerical chemistry and climate
simulation system which uses the Modular Earth Submodel System (MESSy) to
describe tropospheric and middle-atmosphere processes and their interactions
with oceans, land and human influences via dedicated sub-models
<xref ref-type="bibr" rid="bib1.bibx23" id="paren.33"/>.</p>
      <p>The long chemistry climatic simulation RC2-oce-01 <xref ref-type="bibr" rid="bib1.bibx24" id="paren.34"/>,
hereafter referred to as “coupled simulation”, simulates the climate
covering the period 1950–2100. The simulation is performed by the fully
coupled atmosphere–chemistry–ocean model EMAC–MPIOM <xref ref-type="bibr" rid="bib1.bibx38" id="paren.35"/>, using
the 5th generation European Centre Hamburg general circulation model (ECHAM5,
<xref ref-type="bibr" rid="bib1.bibx41" id="altparen.36"/>) as the dynamical core of the atmospheric model and
the MESSy submodel MPIOM (Max Planck Institute Ocean Model,
<xref ref-type="bibr" rid="bib1.bibx29" id="altparen.37"/>) as the dynamical core of the ocean model, which computes
SST and sea ice. The simulation resolution uses a spherical truncation of T42
(corresponding to a quadratic Gaussian grid of approx. <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>2.8</mml:mn><mml:mo>×</mml:mo><mml:mn>2.8</mml:mn></mml:mrow></mml:math></inline-formula><inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> in latitude and longitude) and 47 vertical hybrid pressure
levels up to <inline-formula><mml:math display="inline"><mml:mn>0.01</mml:mn></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> into the middle atmosphere (approximately
<inline-formula><mml:math display="inline"><mml:mn>80</mml:mn></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">km</mml:mi></mml:math></inline-formula> with a resolution of <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn>20</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula> (<inline-formula><mml:math display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">km</mml:mi></mml:math></inline-formula>) at the tropopause), referred to as T42L47MA. This vertical
resolution is essential in order to take into account the influence of the
stratosphere on the NAO variability <xref ref-type="bibr" rid="bib1.bibx1" id="paren.38"/>. Proper representation of
the stratospheric dynamics is important for simulating future climate changes
and a realistic reproduction of the NAO changes <xref ref-type="bibr" rid="bib1.bibx45" id="paren.39"/>.
<xref ref-type="bibr" rid="bib1.bibx44" id="normal.40"/> further showed that the stratospheric variability has to be
reproduced in order for models to fully simulate surface climate variations
in the North Atlantic sector. The resolution for the ocean corresponds to an
average horizontal grid spacing of <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">3</mml:mn><mml:mo>×</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula><inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> with 40 unevenly
spaced vertical levels (GR30L40). An important feature of the EMAC model is
its capability to provide a careful treatment of chemical processes and
dynamical feedbacks through radiation <xref ref-type="bibr" rid="bib1.bibx4" id="paren.41"/>. Thus, the
coupled simulation includes gas-phase species computed online through the
MECCA submodel <xref ref-type="bibr" rid="bib1.bibx42" id="paren.42"/>, while it uses a monthly climatology of
atmospheric aerosols (i.e. monthly aerosol variations are kept constant
throughout the years) to take into account the interactions with radiation
and heterogeneous chemistry. The model incorporates anthropogenic emissions
as a combination of the ACCMIP <xref ref-type="bibr" rid="bib1.bibx27" id="paren.43"/> and RCP 6.0 scenario
<xref ref-type="bibr" rid="bib1.bibx11" id="paren.44"/>. A detailed description can be found in <xref ref-type="bibr" rid="bib1.bibx24" id="normal.45"/> and
references therein. Let us stress that the same EMAC model forced with SST
has been already used by <xref ref-type="bibr" rid="bib1.bibx2" id="normal.46"/> to successfully reproduce the
NAO.</p>
      <p>Coupled general circulation models (GCMs) perform better than atmospheric GCMs forced with SST in reproducing the spatial patterns of atmospheric
low variability and the NAO phenomenon <xref ref-type="bibr" rid="bib1.bibx43" id="paren.47"/>. Several works have
shown that coupled models are able to simulate the main features of the NAO
(e.g. <xref ref-type="bibr" rid="bib1.bibx33 bib1.bibx47" id="altparen.48"/>). Recently, <xref ref-type="bibr" rid="bib1.bibx53" id="normal.49"/> have quantified the
contribution of the coupling in the NAO variability, showing that 20 % of
the NAO monthly variability is caused by the ocean–atmosphere coupling and
80 % is due to the chaotic atmospheric variability. Therefore, a coupled
model is essential for a reasonable projection of future NAO. Our model is
one of the first to include a full dynamical ocean–atmosphere coupling,
stratospheric circulation in conjunction with online chemistry and
anthropogenic emissions, thus providing state-of-the-art simulation
capability of the phenomenon and potential impacts.</p>
      <p>In order to investigate the transport of pollutants we use passive tracers
with emissions modelled after <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula> emissions for the year 2000 (i.e. no
interannual variability) and decay lifetime constant in time. These tracers
are well suited for investigating transport-related effects as no chemical
influences or emission variability are included. <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula> is a good proxy
for anthropogenic pollution, as it is mostly emitted by biomass burning and
human activities <xref ref-type="bibr" rid="bib1.bibx37" id="paren.50"/>. In particular, we consider two passive
<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula> tracers with a constant exponential decay (<inline-formula><mml:math display="inline"><mml:mi>e</mml:mi></mml:math></inline-formula>-folding time) equal
to 25 and 50 days, referred to as <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>50</mml:mn></mml:mrow></mml:math></inline-formula>
respectively. For the whole analysis we focus on the winter (DJF:
December–January–February) seasonal means, since the sea-level pressure
(SLP) amplitude anomalies are larger in winter and the NAO is typically
stronger in this period. To study the intercontinental transport of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula>
(Sect. <xref ref-type="sec" rid="Ch1.S4.SS2"/>) we compute the vertically integrated tracer
transport vector, defined as <xref ref-type="bibr" rid="bib1.bibx18" id="normal.51"/>:
          <disp-formula id="Ch1.E1" content-type="numbered"><mml:math display="block"><mml:mrow><mml:mi mathvariant="bold-italic">Q</mml:mi><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mi>g</mml:mi></mml:mfrac></mml:mstyle><mml:munderover><mml:mo movablelimits="false">∫</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mrow><mml:msub><mml:mi>p</mml:mi><mml:mi mathvariant="normal">s</mml:mi></mml:msub></mml:mrow></mml:munderover><mml:mi>r</mml:mi><mml:mi mathvariant="bold-italic">u</mml:mi><mml:mi mathvariant="normal">d</mml:mi><mml:mi>p</mml:mi><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
        where <inline-formula><mml:math display="inline"><mml:mi>r</mml:mi></mml:math></inline-formula> is the mixing ratio of the tracer (i.e. <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> or
<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>50</mml:mn></mml:mrow></mml:math></inline-formula>) in <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">mol</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:mi mathvariant="bold-italic">u</mml:mi></mml:math></inline-formula> the horizontal wind speed,
<inline-formula><mml:math display="inline"><mml:mi>p</mml:mi></mml:math></inline-formula> the atmospheric pressure, <inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>p</mml:mi><mml:mi mathvariant="normal">s</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> the surface pressure and <inline-formula><mml:math display="inline"><mml:mi>g</mml:mi></mml:math></inline-formula> the
gravitational acceleration.</p>
</sec>
<sec id="Ch1.S3">
  <title>NAO representation and changes</title>
<sec id="Ch1.S3.SS1">
  <title>NAO representation</title>
      <p>In order to define the spatial structure and temporal evolution of the NAO we
use Empirical Orthogonal Function (EOF) analysis. We compute the eigenvectors
of the cross-covariance matrix of the time variations of the SLP
<xref ref-type="bibr" rid="bib1.bibx20" id="paren.52"/>. By definition the eigenvectors are spatially and
temporally mutually orthogonal and scale according to the amount of the total
variance they explain; the leading EOF (EOF1) explains the largest percentage
of the temporal variance in the dataset. The NAO is identified by the EOF1 of
the cross-covariance matrix computed from the SLP anomalies in the North
Atlantic sector. The EOF1 spatial pattern is associated with a north–south
pressure dipole with its centres of action corresponding to the NAO poles
with highest SLP variability. Therefore, we compute the EOF1 from winter
seasonal SLP anomalies in the North Atlantic sector (20–80<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N,
90<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W–40<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) and we find that the long chemistry coupled
simulation (1950–2100) reproduces the NAO signal with the typical
north–south dipole structure (Fig. <xref ref-type="fig" rid="Ch1.F1"/>, top). The EOF1 explains
38.8 % of the total variance, in accordance with the results found in
literature (e.g. <xref ref-type="bibr" rid="bib1.bibx10 bib1.bibx49" id="altparen.53"/>). In order to detect the NAO
differences between the past and the end of the 21st century, we define two
30-year-long periods referred to as “recent past” (1980–2010) and
“future” (2070–2100). Figure <xref ref-type="fig" rid="Ch1.F1"/> (centre and bottom) shows the EOF1
analysis for the two distinct periods. A climatological timescale (30 years)
for the two periods has been chosen to reduce the interdecadal variability.
Additionally, we have chosen various climatological timescales of 30 years
during the past and future and we have computed the EOF1 in all periods, i.e.
1950–1979, 1960–1989, 1970–1999, 1980–2009 in the past and 2040–2069,
2050–2079, 2060–2089, 2070–2099 in the future. The results (shown in
Fig. S1 in the Supplement) exhibit differences between the two periods, past
and future, but not between any of the climatological timescales
within each period. Thus, the changes observed for the past and future NAO
patterns are not due to decadal variability but rather they are climate-induced.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><caption><p>Leading empirical orthogonal function (EOF1) of the winter (DJF)
mean sea-level pressure (SLP) anomalies in the North Atlantic sector
(20–80<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 90<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W–40<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) of the coupled
simulation considering the full period 1950–2100 (top), recent past
period: 1980–2010 (centre), and future period: 2070–2100 (bottom). The
percentage at the top right of each figure quantifies the total variance
explained. The patterns are displayed in terms of amplitude (<inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">hPa</mml:mi></mml:math></inline-formula>),
obtained by regressing the SLP anomalies on the principal component time
series.</p></caption>
          <?xmltex \igopts{width=227.622047pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016-f01.png"/>

        </fig>

      <p>In Fig. <xref ref-type="fig" rid="Ch1.F1"/> we can see that the centres of action of the NAO move north-eastward towards the end of the century.
Such NAO shift is in agreement with the results obtained by <xref ref-type="bibr" rid="bib1.bibx49" id="normal.54"/>,
<xref ref-type="bibr" rid="bib1.bibx17" id="normal.55"/> and <xref ref-type="bibr" rid="bib1.bibx36" id="normal.56"/> for a climate-change global-warming scenario.</p>
      <p>The shift of the NAO centres of action has to be taken into account when
examining the temporal evolution of the NAO pattern. The NAO station-based
index, defined as the difference in the normalized SLP between one northern
station in Iceland and one southern station in the Azores, is fixed in space
and is not able to capture the spatial variability of the NAO centres of
action over seasonal <xref ref-type="bibr" rid="bib1.bibx20" id="paren.57"/> or (future) decadal <xref ref-type="bibr" rid="bib1.bibx49" id="paren.58"/>
scales. Since our model projects a spatial shift of the NAO centres, we will
be considering the principal component time series of the leading EOF of SLP
(PC1) <xref ref-type="bibr" rid="bib1.bibx20" id="paren.59"/> as NAO temporal index. The normalized PC1 computed
for the entire simulation (1950–2100) after subtracting the SLP climatology
of 1980–2010 is shown in Fig. <xref ref-type="fig" rid="Ch1.F2"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><caption><p>Normalized principal component time series (PC1) of the leading empirical orthogonal
function (EOF1) of the winter mean
sea-level pressure (SLP) anomalies for the entire simulation period (1950–2100). The PC1 has been computed after
removing the SLP climatology for the recent past (1980–2010).</p></caption>
          <?xmltex \igopts{width=227.622047pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016-f02.png"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS2">
  <title>NAO changes</title>
      <p>To investigate the NAO temporal variability and trends, we calculate,
considering sliding windows, the linear regression coefficients with respect
to time of the PC1 computed for the entire 150 year simulation
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>). In particular, we define windows of variable length between
a minimum of 10 years and a maximum equal to 150 years sliding along the
whole PC1 time series. We compute the linear slope (trend) for each window
and assign the value to the window central year (e.g. the regression
coefficient of the PC1 series in the selected period 1980–1990, an 11 year
window, is assigned to the year 1985). Results in Fig. <xref ref-type="fig" rid="Ch1.F3"/> show that
no change in the projected future NAO variability is identified compared to
the past when considering periods shorter than 30 years. For windows of
length between 30 and 60 years, upward trends (centred in the 1980s and
2040s) interchange with downward trends (centred in the 2010s and 2060s). On
longer window lengths we find that very weak non-statistically-significant
NAO trends are prevalent. The slope of the overall trend computed for the
entire PC1 is <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mn>2.99</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup><mml:mo>±</mml:mo><mml:mn>0.95</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:msup><mml:mi mathvariant="normal">year</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula>, i.e. significant at 95 %. In
summary, our coupled EMAC–MPIOM model predicts a small significant positive
trend for the NAO (for the 150 year horizon) in agreement with other studies
that have used coupled models (e.g. <xref ref-type="bibr" rid="bib1.bibx14 bib1.bibx17 bib1.bibx47" id="altparen.60"/>). In the
same plot (Fig. <xref ref-type="fig" rid="Ch1.F3"/>), we have marked two triangles in correspondence
to the recent past and future periods, with the aim of stressing the NAO
trend changes. In the lower triangle we distinguish two sharp patterns: an
upward trend (red shading) which dominates between 1980 and 1991 and a
downward trend (blue shading) which dominates from 1992 onwards. Differently,
in the upper triangle we note that, at the end of the century, there is a
clear prevalence of positive NAO trends.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><caption><p>Linear regression coefficients of the PC1 based on coupled
simulation data computed in sliding windows with variable length for the
whole period 1950–2100. Plotted in the <inline-formula><mml:math display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis are the window lengths
expressed in years, and in the <inline-formula><mml:math display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axis the central year of the windows. The
regression coefficient values are expressed in <inline-formula><mml:math display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="normal">year</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> (see colour
legend). Points marked with black crosses indicate the 95 % level of
significance. The green triangles indicate the areas of the two periods,
recent past and future.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016-f03.png"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><caption><p>NAO phase number distributions, computed in the recent past (left) and future
(right) periods.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016-f04.png"/>

        </fig>

      <p>To enhance the analysis of NAO temporal evolution, we compute the number of
(winter) NAO phases over 30 years, in the recent past and in the future
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>). In such a way, we study how the distribution of NAO
phases evolves. In the recent past (Fig. <xref ref-type="fig" rid="Ch1.F4"/>, left) the distribution covers a
large PC1 interval (<inline-formula><mml:math display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn><mml:mo>;</mml:mo><mml:mn>2.5</mml:mn><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula>) and the number of NAO phases is at most <inline-formula><mml:math display="inline"><mml:mn mathvariant="normal">3</mml:mn></mml:math></inline-formula>,
except in the interval <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>;</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula> where it is clearly higher (equal to <inline-formula><mml:math display="inline"><mml:mn mathvariant="normal">9</mml:mn></mml:math></inline-formula> and
<inline-formula><mml:math display="inline"><mml:mn>10</mml:mn></mml:math></inline-formula>). By contrast, in the future (Fig. <xref ref-type="fig" rid="Ch1.F4"/>, right) the distribution
is skewed towards positive values of PC1 (the interval is <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mo>-</mml:mo><mml:mn>1.5</mml:mn><mml:mo>;</mml:mo><mml:mn>2.5</mml:mn><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula>), with
numbers of NAO phases between <inline-formula><mml:math display="inline"><mml:mn mathvariant="normal">4</mml:mn></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mn mathvariant="normal">7</mml:mn></mml:math></inline-formula> in the interval <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mo>-</mml:mo><mml:mn>1.5</mml:mn><mml:mo>;</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula> and
between <inline-formula><mml:math display="inline"><mml:mn mathvariant="normal">1</mml:mn></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mn mathvariant="normal">3</mml:mn></mml:math></inline-formula> in the interval <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>;</mml:mo><mml:mn>2.5</mml:mn><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula>. Therefore, at the end of the
century the number of negative NAO phases increases (15 in the future vs. 10
in the past) and, vice versa, the number of positive NAO phases decreases (16
in the future vs. 21 in the past). However, the “high NAO extreme events”
(PC1 <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn>1.5</mml:mn></mml:mrow></mml:math></inline-formula>) are more frequent in the future (4 in the future vs. 1 in the
past), while the number of “low NAO extreme events” (PC1 <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mo>-</mml:mo><mml:mn>1.5</mml:mn></mml:mrow></mml:math></inline-formula>)
decreases (0 in the future vs. 3 in the past), and such results are
consistent with the future positive trend commented on before.</p>
</sec>
</sec>
<sec id="Ch1.S4">
  <title>NAO effects on tracer transport in the future</title>
<sec id="Ch1.S4.SS1">
  <title>Correlation and regression analysis</title>
      <p>In order to investigate the NAO influence on tracer transport we compute the
correlation (Fig. S2 in the Supplement) and the regression (Fig. <xref ref-type="fig" rid="Ch1.F5"/>)
between the PC1 and tracer mixing ratio at the surface level. We consider
passive tracers whose emissions and decay lifetime are constant
(<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>50</mml:mn></mml:mrow></mml:math></inline-formula>) in order to remove influences by chemical
production and decomposition variability. In this way the
analysis gives information purely on the effect of tracer transport. We
perform the correlation and regression considering the <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> tracer,
which undergoes exponential decay with <inline-formula><mml:math display="inline"><mml:mi>e</mml:mi></mml:math></inline-formula>-folding time equal to 25 days. A
supplementary analysis is repeated for <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>50</mml:mn></mml:mrow></mml:math></inline-formula>, with 50 days
<inline-formula><mml:math display="inline"><mml:mi>e</mml:mi></mml:math></inline-formula>-folding constant, to provide a constraint on the systematic uncertainty
associated with the resident time of the tracer in the atmosphere and to show
the robustness of our results. To identify the future changes in transport
pathways related to the NAO, we perform the analysis separately in the two
periods, recent past and future.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><caption><p>Regression of the winter seasonal <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> mixing ratio anomalies
at surface level against the normalized PC1 computed for the recent past (left) and future (right) periods.
The unit is <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="normal">mol</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">mol</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> and the points marked with a white cross indicate local significance at the 95 %.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016-f05.png"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><caption><p>Differences between future (2070–2100) and recent past (1980–2010) temporal averages of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> winter surface
mixing ratio, both in the case of high NAO (PC1 <inline-formula><mml:math display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> 0.5) (left) and low NAO (PC1 <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:math></inline-formula>.5) (right).
More precisely, plots show the results of <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mo>(</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow><mml:msubsup><mml:mn mathvariant="normal">5</mml:mn><mml:mtext>ave</mml:mtext><mml:mtext>fut</mml:mtext></mml:msubsup><mml:mo>-</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow><mml:msubsup><mml:mn mathvariant="normal">5</mml:mn><mml:mtext>ave</mml:mtext><mml:mtext>past</mml:mtext></mml:msubsup><mml:mo>)</mml:mo><mml:mo>/</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow><mml:msubsup><mml:mn mathvariant="normal">5</mml:mn><mml:mtext>ave</mml:mtext><mml:mtext>past</mml:mtext></mml:msubsup><mml:mo>]</mml:mo><mml:mo>×</mml:mo><mml:mn>100</mml:mn></mml:mrow></mml:math></inline-formula>, so
the coloured bars indicate the percentages.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016-f06.png"/>

        </fig>

      <p>By means of the correlation (Fig. S2) we determine where European and eastern
USA CO-like tracers have a linear relationship with NAO. The higher the
correlation (in absolute value), the stronger the linear dependence between
tracer mixing ratio and PC1. We observe that, in the recent past, the PC1 and
<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> mixing ratio are significantly correlated over the northern
part of the northern American east coast, the north-western Baffin Bay
region, the Arctic, northern Africa and part of the Iberian Peninsula. Also present is a
continuous area of significant anti-correlation encompassing the American
central-east coast (near Florida and Cuba), through the central North
Atlantic Ocean, towards northern and eastern Europe, and the Black Sea
regions. The analysis with <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>50</mml:mn></mml:mrow></mml:math></inline-formula> leads to similar results (Fig. S3 in the
Supplement),
and thus the outcomes can be considered robust under the uncertainties
associated with pollutant tracer atmospheric residence lifetimes. Since the
CO concentration over Europe is mostly influenced by emissions from Europe
and only partially from North America (the Asian contribution can be
considered negligible, <xref ref-type="bibr" rid="bib1.bibx6" id="altparen.61"/>), we can compare our results with
the findings of <xref ref-type="bibr" rid="bib1.bibx2" id="normal.62"/> that used tracers tagged by origin. We
find that the transport pattern in the recent past is similar to the one of
<xref ref-type="bibr" rid="bib1.bibx2" id="normal.63"/> for European emissions. However, our results supersede
those in <xref ref-type="bibr" rid="bib1.bibx2" id="normal.64"/> as that study was limited in the period
1960–2010 and was forced by prescribed SST and global atmospheric hydroxyl
radical (<inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">OH</mml:mi></mml:mrow></mml:math></inline-formula>) concentrations (as the removal mechanism for <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula>
depletion). As far as the future period is concerned, all significantly
correlated areas increase in size compared to the past, except for the area north-west of the Baffin Bay which decreases. The area with positive
correlation over the Arctic spreads southwards up to the Scandinavian
Peninsula and the one over Africa spreads westwards and northwards, covering
further the Iberian Peninsula. Moreover, the correlation over north-western
Africa and the nearby ocean becomes stronger with values between <inline-formula><mml:math display="inline"><mml:mn>0.6</mml:mn></mml:math></inline-formula> and
<inline-formula><mml:math display="inline"><mml:mn>1.0</mml:mn></mml:math></inline-formula> – greater than in the past. Similarly, the area with significant
anti-correlation is also wider with respect to the past, and the magnitude of the
negative correlation increases over north-eastern Europe, southern Scandinavia,
and the North Atlantic Ocean (between Great Britain and Iceland) with values
in the range <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn>0.6</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn>0.8</mml:mn></mml:mrow></mml:math></inline-formula>. Again, the analysis considering <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>50</mml:mn></mml:mrow></mml:math></inline-formula>
has produced similar results.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><caption><p>Temporal averages of vertically integrated <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> tracer transport vectors
(<inline-formula><mml:math display="inline"><mml:mrow><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mi mathvariant="normal">mol</mml:mi><mml:mi mathvariant="normal">mol</mml:mi></mml:mfrac></mml:mstyle><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mi mathvariant="normal">kg</mml:mi><mml:mrow><mml:mi mathvariant="normal">m</mml:mi><mml:mo>⋅</mml:mo><mml:mi mathvariant="normal">s</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:math></inline-formula>) for winters with high NAO
(PC1 <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:math></inline-formula>.5) (top) and low NAO (PC1 <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:math></inline-formula>.5) (bottom), both in the recent past (left)
and in the future (right). </p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/15581/2016/acp-16-15581-2016-f07.png"/>

        </fig>

      <p>In order to better define the relationship between NAO and tracer transport,
we regress the <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> mixing ratio against the normalized PC1
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>). Analogously to the correlation, areas with positive values
mean that positive/negative NAO phases drive a higher/lower stagnation of
trace pollutants, while areas with negative values mean that
positive/negative NAO phases drive a depletion/increment of such pollutants.
However, in contrast to the correlation, the regression map shows how
intense the effect of NAO on <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> concentration could be. We observe
that correlation and regression patterns are very similar. The regression
analysis shows that the flow over Europe transports tracers over the Arctic,
southern Mediterranean, and Africa during positive NAO phases and splits the
European continent in two distinct areas. Conversely, during negative NAO
phases, the air is more stagnant over central Europe, allowing pollutants to
accumulate. Such results extend what has been found by <xref ref-type="bibr" rid="bib1.bibx3" id="normal.65"/>,
<xref ref-type="bibr" rid="bib1.bibx7" id="normal.66"/> and <xref ref-type="bibr" rid="bib1.bibx2" id="normal.67"/>, who analysed the NAO effects on
ozone, carbon monoxide and origin-tagged idealized tracers, respectively. The
difference between the future regression and the recent past regression is
computed for a clear comparison of the two periods (Fig. S4). We find that
the dichotomy over Europe is further stressed in the future, which is mostly
characterized by positive NAO trends (Fig. <xref ref-type="fig" rid="Ch1.F3"/>) and more “high NAO
extreme events” (Fig. <xref ref-type="fig" rid="Ch1.F4"/>) with respect to the past. Indeed, a
stronger Azores High (during positive NAO) leads to enhanced transatlantic
transport towards north-eastern Europe and then southwards, over Africa, and to
a stronger separation of the flow over Europe. Therefore, northward transport
to the Arctic and southward transport to Africa are further enhanced in the
future. Such considerations are confirmed when studying the differences
between future and recent past tracer concentration and transport (see next
subsection).</p>
      <p>Consequently, at the end of the century, the south-western Mediterranean and
northern Africa will suffer from higher pollutant concentrations during
positive NAO phases compared to the past, while a wider part of northern
Europe will benefit from lower concentrations of long-range pollutants
(associated with improved surface air quality) during the positive NAO phases
with respect to the past. Similarly, the splitting over the American east
coast will be enhanced as well, to a lesser degree. Nevertheless, we should
note that this work is related only to the transport of CO-like tracers with
constant lifetime and emissions, and thus it does not account for a possible
(and probable) decrease of pollutant emissions both over Northern America and
in Europe. Moreover, we do not deal with the reduction of aerosol and aerosol
precursors emissions, predicted by most of the representative concentration
pathways (RCPs,
<xref ref-type="bibr" rid="bib1.bibx26" id="altparen.68"/>) over the Mediterranean, since we focus on trace gases
rather than aerosols.</p>
</sec>
<sec id="Ch1.S4.SS2">
  <title>Tracer transport changes</title>
      <p>Here, we further develop our analysis differentiating high and low
NAO events, both in the recent past and in the future.
We define “high NAO” and “low NAO”
as (winter) periods with PC1 higher than <inline-formula><mml:math display="inline"><mml:mn>0.5</mml:mn></mml:math></inline-formula> and lower than <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn>0.5</mml:mn></mml:mrow></mml:math></inline-formula>, respectively.
We obtain 12 high and 8 low NAO phases in the recent past and
9 high and 11 low NAO phases in the future. The averages of the PC1 amplitudes (all computed over
at least 8 values) are equal to <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn>1.38</mml:mn></mml:mrow></mml:math></inline-formula> in the recent past and <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn>1.01</mml:mn></mml:mrow></mml:math></inline-formula> in the future considering the
low NAO events and equal to <inline-formula><mml:math display="inline"><mml:mn>0.83</mml:mn></mml:math></inline-formula> in the recent past and <inline-formula><mml:math display="inline"><mml:mn>1.24</mml:mn></mml:math></inline-formula> in the future considering
the high NAO events.
Thus, we note that in the future the events categorized
as high will have, on average, a higher PC1 amplitude than those in the recent past and,
similarly, the future events categorized as low will be less negative than
those in the recent past.
Therefore, we find that the number of low/high NAO events will increase/decrease
in the future, while the mean PC1 amplitudes will increase in the future in both cases
(low and high NAO).</p>
      <p>Firstly, we compute the temporal averages of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> winter surface
mixing ratio during high and low NAO events in order to investigate how
tracer concentration changes in the future. In Fig. <xref ref-type="fig" rid="Ch1.F6"/> we show the
differences (percentages) between future and recent past during high and low
NAO periods. We observe that in the future, during high NAO
(Fig. <xref ref-type="fig" rid="Ch1.F6"/>, left), concentrations increase by 10 % over northern Africa and the Mediterranean and even by 15 % over some areas of the Iberian
Peninsula, Greece and the Aegean Sea; concentrations are lower than in the past
over northern Europe and Greenland (in the range down to <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn>10</mml:mn></mml:mrow></mml:math></inline-formula> %). On the
other hand, during low NAO (Fig. <xref ref-type="fig" rid="Ch1.F6"/>, right) <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula>
concentrations increase over north-eastern Africa and west-central Europe (up to
15 %) and decrease over northern Scandinavia, the Arctic, and some areas of
North America and the Atlantic Ocean (down to <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn>10</mml:mn></mml:mrow></mml:math></inline-formula> %). Such variations are
likely due to the more positive NAO events in the future. With this analysis
we corroborate the results of the previous subsection and, moreover, we
estimate which concentration changes are associated with the different NAO
phases. Nevertheless, we would like to stress that, while the correlation and
regression analyses were performed over 30 years, here fewer years are considered (having to satisfy the conditions PC1 <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mo>-</mml:mo><mml:mn>0.5</mml:mn></mml:mrow></mml:math></inline-formula> or PC1 <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn>0.5</mml:mn></mml:mrow></mml:math></inline-formula>).</p>
      <p>Secondly, following the same definitions of high and low NAO, we compute the temporal averages of <inline-formula><mml:math display="inline"><mml:mi mathvariant="bold-italic">Q</mml:mi></mml:math></inline-formula> (<xref ref-type="disp-formula" rid="Ch1.E1"/>).
The main features of transport are in agreement with <xref ref-type="bibr" rid="bib1.bibx18" id="normal.69"/> and <xref ref-type="bibr" rid="bib1.bibx2" id="normal.70"/>:
during positive NAO (Fig. <xref ref-type="fig" rid="Ch1.F7"/>, top) the axis of maximum transport has a southwest-to-northeast orientation
across the Atlantic and extends farther to north-eastern Europe, while during negative NAO (Fig. <xref ref-type="fig" rid="Ch1.F7"/>, bottom) it is
more longitudinally oriented.
Comparing the recent past and future, we observe that during high NAO (Fig. <xref ref-type="fig" rid="Ch1.F7"/>, top) the east-northward
transport of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> is more pronounced in the future over
the North Atlantic Ocean, from the northern American coast towards Ireland, while it gets weaker over
southern Greenland, the Mediterranean and western Europe.
During low NAO (Fig. <xref ref-type="fig" rid="Ch1.F7"/>, bottom), the eastward <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> transport over the North Atlantic
Ocean extends farther eastwards in the future,
while it decreases over the Mediterranean Sea and north-eastern Africa; in contrast to the high NAO case,
transport gets slightly stronger over southern Greenland in the future.
For a more immediate comparison we have also computed the differences between the two periods and the
results are shown in Fig. S5.
The main future changes of <inline-formula><mml:math display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi><mml:mi mathvariant="normal">_</mml:mi><mml:mn>25</mml:mn></mml:mrow></mml:math></inline-formula> transport, which gets generally stronger over the North Atlantic Ocean
and weaker over the Mediterranean, confirm information retrieved from the correlation and regression analysis.</p>
</sec>
</sec>
<sec id="Ch1.S5" sec-type="conclusions">
  <title>Conclusions</title>
      <p>A free-running simulation performed by the coupled EMAC–MPIOM model
has been analysed in order to study the influence of the NAO on future pollutant
transport and concentration changes.
The simulation takes into account the GHG increment during the 21st century according to the
ACCMIP <xref ref-type="bibr" rid="bib1.bibx27" id="paren.71"/> and RCP 6.0 scenario <xref ref-type="bibr" rid="bib1.bibx11" id="paren.72"/> and uses a monthly aerosol climatology.
The model is able to reproduce the SLP anomalies and the NAO signal <xref ref-type="bibr" rid="bib1.bibx2" id="paren.73"/>, and
the EOF analysis performed with the coupled simulation shows the typical dipole pattern which is
identified as the NAO.</p>
      <p>Similarly to other coupled GCMs, when considering the full modelled period in
a global-warming scenario, our model projects (i) a northeastward shift of
the NAO centres of action (<xref ref-type="bibr" rid="bib1.bibx49 bib1.bibx17 bib1.bibx36" id="altparen.74"/>) and (ii) a very
weak but significant positive trend of the NAO
(<xref ref-type="bibr" rid="bib1.bibx17 bib1.bibx14 bib1.bibx47" id="altparen.75"/>). This suggests that the
anthropogenic forcing has a non-null contribution in the NAO evolution.
Moreover, in our model the NAO trends computed over periods shorter than
30 years will continue to oscillate between positive and negative values in
the future. The analysis of the NAO phase distribution reveals an increase of
the negative NAO frequencies in the future although with much reduced
amplitudes. On the contrary, positive NAO phases do decrease in frequency but
increase in amplitude.</p>
      <p>As far as the NAO impact on tracer transport is concerned, our results show
that, in the recent past, NAO affected surface tracer concentrations with
increased tracer concentrations over the Arctic, southern Mediterranean and
northern Africa during positive NAO (similarly to the findings of
<xref ref-type="bibr" rid="bib1.bibx3 bib1.bibx7 bib1.bibx2" id="altparen.76"/>). Considering CO-like tracers with
constant lifetime and emissions, we find that, at the end of the century, the
NAO effects on pollutants will be enhanced, i.e. tracer concentrations over
those areas where they are depleted during positive NAO will reduce more,
while they will increase over those areas to which they are transported. This
means that tracers will be transported more efficiently towards those areas
which already suffer from bad air-quality conditions during positive NAO,
i.e. over the Arctic, southern Mediterranean and Africa.</p>
      <p>Such conclusions are also confirmed by the computation of tracer mixing ratios
and transport in the Atlantic sector during high positive and low negative NAO phases.
Future tracer concentrations during positive NAO will increase over central Europe,
the southern Mediterranean and northern Africa, and reduce over northern
Europe and Greenland. Both the NAO amplitude changes and the NAO shift contribute
to such concentration variations. For positive NAO, future tracer transport with respect to the past
will get generally stronger over the North Atlantic Ocean and weaker over
the Mediterranean region,
enhancing the depletion of  pollutants from central-northern Europe and
the stagnation over the southern Mediterranean and northern Africa.
We remind that these results refer to constant emissions and idealized tracers (i.e. constant
decay time).</p>
</sec>
<sec id="Ch1.S6">
  <title>Data availability</title>
      <p>The analysed data are the results of one simulation (RC2-oce-01) described in
Jöckel et al. (2016). All simulations of Jöckel et al. (2016) will be
available in the Climate and Environmental Retrieval and Archive (CERA)
database at the German Climate Computing Centre (DKRZ;
<uri>http://cerawww.dkrz.de/WDCC/ui/Index.jsp</uri>). The corresponding digital
object identifiers (DOI) will be published on the MESSy consortium web-page
(<uri>http://www.messy-interface.org</uri>).</p><?xmltex \hack{\newpage}?>
</sec>

      
      </body>
    <back><app-group>
        <supplementary-material position="anchor"><p><bold>The Supplement related to this article is available online at <inline-supplementary-material xlink:href="http://dx.doi.org/10.5194/acp-16-15581-2016-supplement" xlink:title="pdf">doi:10.5194/acp-16-15581-2016-supplement</inline-supplementary-material>.</bold></p></supplementary-material>
        </app-group><ack><title>Acknowledgements</title><p>The authors wish to extend their gratitude to the MESSy Consortium and the
international IGAC/SPARC Chemistry–Climate Model Initiative <xref ref-type="bibr" rid="bib1.bibx9" id="paren.77"/>.
The analysed simulations were carried out as part of the Earth System
Chemistry integrated Modelling (ESCiMo) project at the German Climate Computing Centre (Deutsches
Klimarechenzentrum, DKRZ). DKRZ and its scientific steering committee are
gratefully acknowledged for providing the required computational
resources.<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>The article processing charges for
this open-access <?xmltex \hack{\newline}?> publication were covered by the Max Planck
Society. <?xmltex \hack{\newline}?><?xmltex \hack{\newline}?> Edited by: P. Haynes <?xmltex \hack{\newline}?>
Reviewed by: two anonymous referees</p></ack><ref-list>
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<abstract-html><p class="p">The North Atlantic Oscillation (NAO) plays an important role in the climate
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concentrations. Such results are confirmed by the changes observed in the
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