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  <front>
    <journal-meta><journal-id journal-id-type="publisher">ACP</journal-id><journal-title-group>
    <journal-title>Atmospheric Chemistry and Physics</journal-title>
    <abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys.</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">1680-7324</issn><publisher>
    <publisher-name>Copernicus Publications</publisher-name>
    <publisher-loc>Göttingen, Germany</publisher-loc>
  </publisher></journal-meta>
    <article-meta>
      <article-id pub-id-type="doi">10.5194/acp-20-15285-2020</article-id><title-group><article-title>Weaker cooling by aerosols due to dust–pollution interactions</article-title><alt-title>Weaker cooling by aerosols</alt-title>
      </title-group><?xmltex \runningtitle{Weaker cooling by aerosols}?><?xmltex \runningauthor{K.~Klingm\"{u}ller et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Klingmüller</surname><given-names>Klaus</given-names></name>
          <email>k.klingmueller@mpic.de</email>
        <ext-link>https://orcid.org/0000-0002-8425-8150</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Karydis</surname><given-names>Vlassis A.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1616-9746</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Bacer</surname><given-names>Sara</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-0052-1968</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Stenchikov</surname><given-names>Georgiy L.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-9033-4925</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff5">
          <name><surname>Lelieveld</surname><given-names>Jos</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6307-3846</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Max Planck Institute for Chemistry, Hahn-Meitner-Weg 1, 55128 Mainz, Germany</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Forschungszentrum Jülich GmbH, IEK-8, 52425 Jülich, Germany</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>LEGI, Université Grenoble Alpes, CNRS, Grenoble INP, Grenoble, France</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>The Cyprus Institute, P.O. Box 27456, 1645 Nicosia, Cyprus</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Klaus Klingmüller (k.klingmueller@mpic.de)</corresp></author-notes><pub-date><day>9</day><month>December</month><year>2020</year></pub-date>
      
      <volume>20</volume>
      <issue>23</issue>
      <fpage>15285</fpage><lpage>15295</lpage>
      <history>
        <date date-type="received"><day>30</day><month>May</month><year>2020</year></date>
           <date date-type="rev-request"><day>23</day><month>June</month><year>2020</year></date>
           <date date-type="rev-recd"><day>8</day><month>October</month><year>2020</year></date>
           <date date-type="accepted"><day>20</day><month>October</month><year>2020</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2020 </copyright-statement>
        <copyright-year>2020</copyright-year>
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://acp.copernicus.org/articles/.html">This article is available from https://acp.copernicus.org/articles/.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/.pdf</self-uri>
      <abstract><title>Abstract</title>
    <p id="d1e144">The interactions between aeolian dust and anthropogenic air pollution, notably  chemical ageing of mineral dust and coagulation of dust and pollution
particles, modify the atmospheric aerosol composition and burden. Since the
aerosol particles can act as cloud condensation nuclei, this affects  the radiative transfer not only directly via aerosol–radiation interactions, but also  indirectly through cloud adjustments. We study both radiative effects using
the global ECHAM/MESSy atmospheric chemistry-climate model (EMAC) which
combines the Modular Earth Submodel System (MESSy) with the European
Centre/Hamburg (ECHAM) climate model. Our simulations show that
dust–pollution–cloud interactions reduce the condensed water path and hence  the reflection of solar radiation. The associated climate warming outweighs
the cooling that the dust–pollution interactions exert through the direct  radiative effect. In total, this results in a net warming by dust–pollution
interactions which moderates the negative global anthropogenic aerosol forcing
at the top of the atmosphere by (0.2 <inline-formula><mml:math id="M1" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1) W m<inline-formula><mml:math id="M2" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e175">A prime objective of current atmospheric and climate science is the deeper
understanding of ambient aerosols and their interactions with clouds. This is
motivated by their central role in two areas of societal importance, public
health and climate change. The inhalation of aerosols allows fine particles to
enter deep into the respiratory system or even translocate through the lungs
into the cardiovascular system, causing a multitude of health challenges and making exposure to fine particulate air pollution one of the main public
health risks worldwide <xref ref-type="bibr" rid="bib1.bibx35 bib1.bibx36 bib1.bibx37 bib1.bibx8" id="paren.1"/>.  On the other
hand, aerosols modify the albedo of the Earth, predominantly increasing the
reflection of solar radiation and thus cooling the planet.  Since the emissions
of anthropogenic greenhouse gases are accompanied by those of aerosols, to a
large extent through common source categories, the greenhouse warming has been
partially masked by the aerosol effects on climate <xref ref-type="bibr" rid="bib1.bibx18 bib1.bibx36" id="paren.2"/>.</p>
      <p id="d1e184">The planetary albedo can be increased both directly by interactions of the
anthropogenic aerosol particles with solar radiation and indirectly by enhanced
cloudiness or cloud brightness caused by aerosol particles acting as cloud
condensation nuclei. These direct and indirect effects are estimated to
contribute a negative effective radiative forcing (ERF) of
<inline-formula><mml:math id="M3" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.45 W m<inline-formula><mml:math id="M4" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> each, adding up to about <inline-formula><mml:math id="M5" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.9 W m<inline-formula><mml:math id="M6" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
<xref ref-type="bibr" rid="bib1.bibx18" id="paren.3"/>.</p>
      <p id="d1e228">Since not all aerosols in the atmosphere are of anthropogenic origin – in fact
natural aerosols including aeolian dust and sea salt are the most abundant
components by mass – the anthropogenic pollutants form a mixture with natural
aerosols. On the one hand particulate pollution coagulates with natural
particles and on the other hand natural particles are exposed to chemical
ageing.  <xref ref-type="bibr" rid="bib1.bibx31" id="text.4"/> showed that the interactions between natural
mineral dust and anthropogenic pollution enhance the global net cooling through the direct radiative effects and have a significant impact on regional radiative
transfer. Here we extend the analysis to include the indirect radiative effects.
The abundant atmospheric water vapour represents a vast source of cloud<?pagebreak page15286?> water so
that cloud optical depths are typically much larger than aerosol optical depths.
Therefore, cloud adjustments potentially leverage the aerosol radiative effect, and we may expect the indirect radiative effect of the dust–pollution interactions to be even more significant than the direct effect.</p>
      <p id="d1e234">We use the global ECHAM/MESSy atmospheric chemistry-climate model (EMAC) which
combines the Modular Earth Submodel System (MESSy) with the European
Centre/Hamburg (ECHAM) climate model.  It includes implementations of an
extensive set of relevant physical and chemical processes, including detailed
parametrisations of mineral dust ageing, cloud droplet activation and ice
crystal formation in cirrus and mixed-phase clouds.</p>
      <p id="d1e238">The model and its configuration are described in Sect. <xref ref-type="sec" rid="Ch1.S2"/> followed
by an outline of the methodology of our analysis in Sect. <xref ref-type="sec" rid="Ch1.S3"/>.
Results for the dust–pollution interaction effect on the cloud condensate are presented in Sect. <xref ref-type="sec" rid="Ch1.S4"/> and the resulting effects on radiative transfer in Sect. <xref ref-type="sec" rid="Ch1.S5"/>. Conclusions are presented in
Sect. <xref ref-type="sec" rid="Ch1.S6"/>.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Model description</title>
      <p id="d1e259">The EMAC model version and configuration used in the present study are largely
identical to those used by <xref ref-type="bibr" rid="bib1.bibx30 bib1.bibx31" id="text.5"/>, combining
ECHAM 5.3.02 and MESSy 2.52. However, to allow decadal simulations, the
horizontal resolution has been reduced to a Gaussian T63 grid with a grid
spacing of <inline-formula><mml:math id="M7" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.875</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> along latitudes and about <inline-formula><mml:math id="M8" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.86</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> along
longitudes, corresponding to an edge length of the individual grid cells of
around 200 km or less. The number of vertical levels remains at 31. Moreover,
the present study uses the EDGARv4.3 (Emissions Database for Global Atmospheric
Research) database for anthropogenic emissions <xref ref-type="bibr" rid="bib1.bibx9" id="paren.6"/> and a
back port of the CLOUD submodel from MESSy 2.54 to benefit from recent improvements of the cloud parametrisations.</p>
      <p id="d1e292">As in the previous studies, the GFEDv3.1 (Global Fire Emissions Database)
<xref ref-type="bibr" rid="bib1.bibx53" id="paren.7"/> and AeroCom (Aerosol Comparisons between
Observations and Models) <xref ref-type="bibr" rid="bib1.bibx11" id="paren.8"/> databases provide biomass
burning and sea salt emissions, respectively. Mineral dust emissions are
calculated online by the submodel ONEMIS <xref ref-type="bibr" rid="bib1.bibx25" id="paren.9"/> using the dust
emission scheme presented by <xref ref-type="bibr" rid="bib1.bibx30" id="text.10"/> which is based on
<xref ref-type="bibr" rid="bib1.bibx4" id="text.11"/>.  It differentiates the <inline-formula><mml:math id="M9" display="inline"><mml:mrow><mml:msup><mml:mtext>Ca</mml:mtext><mml:mrow><mml:mo>+</mml:mo><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, K<inline-formula><mml:math id="M10" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>,
<inline-formula><mml:math id="M11" display="inline"><mml:mrow><mml:msup><mml:mtext>Mg</mml:mtext><mml:mrow><mml:mo>+</mml:mo><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M12" display="inline"><mml:mrow><mml:msup><mml:mtext>Na</mml:mtext><mml:mo>+</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> fractions in mineral particles originating
from different deserts <xref ref-type="bibr" rid="bib1.bibx21" id="paren.12"/>.</p>
      <p id="d1e362">The MESSy submodels most relevant for aerosols include the Global Modal Aerosol
Extension (GMXe) <xref ref-type="bibr" rid="bib1.bibx51 bib1.bibx52" id="paren.13"/>. It simulates the
microphysics of four soluble (nucleation, Aitken, accumulation, coarse) and
three insoluble (Aitken, accumulation, coarse) aerosol log-normal modes with
fixed geometric standard deviations (<inline-formula><mml:math id="M13" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="normal">g</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> for the coarse
modes, <inline-formula><mml:math id="M14" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="normal">g</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1.59</mml:mn></mml:mrow></mml:math></inline-formula> for all others).  The count median dry radius
of each mode can vary between fixed boundaries at 6, 60 nm and 1 <inline-formula><mml:math id="M15" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m.  Super
coarse mineral dust particles are therefore only included as part of the coarse
modes with mean radius larger than 1 <inline-formula><mml:math id="M16" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, and their mass is probably underrepresented <xref ref-type="bibr" rid="bib1.bibx3" id="paren.14"/>.  However, their role in the
dust–pollution–cloud interactions is limited by their low number concentration, corresponding to a low probability of pollution particles coagulating with
them, and a comparably short atmospheric residence time, leaving less time for
chemical ageing.</p>
      <p id="d1e418">Within GMXe, the gas–aerosol partitioning can be computed by ISORROPIA II <xref ref-type="bibr" rid="bib1.bibx15" id="paren.15"/> or EQSAM4clim (Equilibrium Simplified Aerosol Model V4
for climate simulations) <xref ref-type="bibr" rid="bib1.bibx46" id="paren.16"/>; here we use ISORROPIA II. Assuming diffusion-limited condensation, it calculates the amount of gas kinetically able to condense using the accommodation coefficients in Table S1 in
the Supplement.  Subsequently the mass is re-distributed between the gas and
aerosol phases to obtain the amount of condensed material <xref ref-type="bibr" rid="bib1.bibx51 bib1.bibx52" id="paren.17"/>.  This means that gaseous compounds
from anthropogenic pollution, including sulfuric acid, nitric acid, hydrochloric acid and ammonia, can condense on mineral dust particles and
initiate their chemical ageing, which is the primary interaction between mineral dust and gaseous pollution, primarily through reactions of acids with mineral
cations.</p>
      <p id="d1e431">Insoluble particles are transferred to the soluble modes if sufficient
hydrophilic material has accumulated to cover the particles with 10 molecular monolayers or if they coagulate with soluble particles <xref ref-type="bibr" rid="bib1.bibx62 bib1.bibx56 bib1.bibx51 bib1.bibx52" id="paren.18"/>.  In particular, freshly emitted mineral dust is assumed to
be hydrophobic and thus emitted into the insoluble aerosol modes (at approximately 89 %, the majority of the mass is emitted into the coarse mode
and the remainder into the accumulation mode), but chemical ageing can transfer
the mineral dust particles to soluble modes.  The chemical ageing and
partitioning of organic aerosol compounds are implemented in the submodel ORACLE (Organic Aerosol Composition and Evolution) <xref ref-type="bibr" rid="bib1.bibx60 bib1.bibx61" id="paren.19"/>. GMXe and ORACLE interact with the gas phase, for which the chemistry is simulated by the submodel MECCA (Module Efficiently Calculating the
Chemistry of the Atmosphere) <xref ref-type="bibr" rid="bib1.bibx55" id="paren.20"/>.</p>
      <p id="d1e443">In addition to the condensation of hydrophilic compounds, the coagulation with soluble particles also transfers insoluble particles to the soluble modes.
Within GMXe, coagulation is implemented following <xref ref-type="bibr" rid="bib1.bibx62" id="text.21"/>
using the coagulation coefficient equation from <xref ref-type="bibr" rid="bib1.bibx16" id="text.22"/>. All
aerosol components are affected by coagulation irrespective of their sources and
their chemical composition, including components represented by “bulk”
tracers, which are treated as chemically inert, and the major particulate
pollutants black carbon, organic compounds, sulfates, nitrate and ammonium. This makes coagulation the primary interaction between mineral dust and
particulate pollution.  Aside from<?pagebreak page15287?> modifying the composition and hygroscopicity
of dust particles, it has a significant effect on the burden of particulate
pollution.  Because typically mineral dust particles are coarser than pollution
particles like soot or sulfate particles, coagulation with dust transfers fine particulate pollution to coarser modes, decreasing the number concentration, especially in the fine modes.  Once in the coarse mode, the pollution is
affected by the shorter atmospheric residence time of coarse particles, which
reduces the mass concentration of particulate pollutants.  After being
transferred to the hydrophilic modes, mineral dust particles grow by taking up
water and act as cloud condensation nuclei. The hygroscopic growth increases the
deposition rate and affects the optical properties.</p>

<table-wrap id="Ch1.T1" specific-use="star"><?xmltex \currentcnt{1}?><label>Table 1</label><caption><p id="d1e454">Globally averaged annual mean cloud properties and contributions
thereto, based on the SST simulations. “Total” represents the simulation
with all emissions, “Mineral dust” and “Anthropogenic pollution” include
the effect of dust–pollution interactions (<inline-formula><mml:math id="M17" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>x</mml:mi></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M18" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">pol</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>x</mml:mi></mml:mrow></mml:math></inline-formula> in
Eq. <xref ref-type="disp-formula" rid="Ch1.E1"/>), and “Dust–pollution interactions” are given by the  interaction term <inline-formula><mml:math id="M19" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>x</mml:mi></mml:mrow></mml:math></inline-formula>, Eq. (<xref ref-type="disp-formula" rid="Ch1.E2"/>).  The  corresponding results from the nudged simulations are provided in Table S4 in
the Supplement.</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="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Total</oasis:entry>
         <oasis:entry colname="col3">Mineral dust</oasis:entry>
         <oasis:entry colname="col4">Anthropogenic pollution</oasis:entry>
         <oasis:entry colname="col5">Dust–pollution interactions</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Droplet number/m<inline-formula><mml:math id="M20" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">(5.845 <inline-formula><mml:math id="M21" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.009) <inline-formula><mml:math id="M22" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math id="M23" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">(<inline-formula><mml:math id="M24" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>2.2 <inline-formula><mml:math id="M25" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1) <inline-formula><mml:math id="M26" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math id="M27" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">9</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4">(5.1 <inline-formula><mml:math id="M28" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1) <inline-formula><mml:math id="M29" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math id="M30" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">9</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col5">(<inline-formula><mml:math id="M31" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>2.2 <inline-formula><mml:math id="M32" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1) <inline-formula><mml:math id="M33" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math id="M34" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">9</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Liquid water path/(g m<inline-formula><mml:math id="M35" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>)</oasis:entry>
         <oasis:entry colname="col2">85.5 <inline-formula><mml:math id="M36" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M37" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.5 <inline-formula><mml:math id="M38" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1</oasis:entry>
         <oasis:entry colname="col4">1.6 <inline-formula><mml:math id="M39" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.2</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M40" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.5 <inline-formula><mml:math id="M41" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.2</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Ice water path/(g m<inline-formula><mml:math id="M42" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>)</oasis:entry>
         <oasis:entry colname="col2">14.70 <inline-formula><mml:math id="M43" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M44" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.04 <inline-formula><mml:math id="M45" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>
         <oasis:entry colname="col4">0.60 <inline-formula><mml:math id="M46" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M47" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.02 <inline-formula><mml:math id="M48" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d1e828">The AEROPT (AERosol OPTical properties) submodel <xref ref-type="bibr" rid="bib1.bibx33 bib1.bibx28" id="paren.23"/> calculates the aerosol optical properties assuming the aerosol
components within each mode to be well mixed in spherical particles with a volume-averaged refractive index.  The refractive indices considered by AEROPT for the
individual components are compiled from the OPAC 3.1 database
<xref ref-type="bibr" rid="bib1.bibx17" id="paren.24"/> (black carbon, mineral dust), the HITRAN 2004 database
<xref ref-type="bibr" rid="bib1.bibx54" id="paren.25"/> (organic carbon, sea salt, ammonium sulfate, water), <xref ref-type="bibr" rid="bib1.bibx26" id="text.26"/> (organic carbon for <inline-formula><mml:math id="M49" display="inline"><mml:mrow><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.7</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M50" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m)
and additional mineral dust values for <inline-formula><mml:math id="M51" display="inline"><mml:mrow><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">2.5</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M52" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m. The full
dataset is specified in the Supplement of <xref ref-type="bibr" rid="bib1.bibx28" id="text.27"/>. The imaginary
part of the dust refractive index provided by the OPAC dataset attains a minimum
of <inline-formula><mml:math id="M53" display="inline"><mml:mrow><mml:mn mathvariant="normal">4</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> at visible and near-infrared wavelengths.  This is lower
than the former recommendation by the World Meteorological Organisation of <inline-formula><mml:math id="M54" display="inline"><mml:mrow><mml:mn mathvariant="normal">8</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx10" id="paren.28"/>, but even smaller and regionally varying
values are found in more recent literature <xref ref-type="bibr" rid="bib1.bibx23 bib1.bibx48 bib1.bibx12" id="paren.29"/>.  Even though a larger
imaginary part of the refractive index corresponds to stronger absorption, we
obtain a distinctive negative climate forcing attributed to mineral dust
(Table <xref ref-type="table" rid="Ch1.T2"/>). In our simulations the modelled dust is usually
internally mixed with other components, and especially water, so that the effective imaginary refractive index of the entire particles is often lower than
the value assumed for pure dust. Using a smaller value for pure dust would
further enhance the negative direct forcing of dust and to some extent the
direct forcing through the dust–pollution interactions. However, the dominant indirect effect of the interactions would not be affected.</p>
      <p id="d1e932">The aerosol optical properties are considered by the radiative transfer submodel
RAD <xref ref-type="bibr" rid="bib1.bibx14" id="paren.30"/> to account for the aerosol–radiation coupling.  In the solar spectrum, absorption and scattering are computed using extinction
coefficient, single scattering albedo and asymmetry parameter, whereas in the
terrestrial spectrum scattering is neglected. The latter approximation is valid
for particles much smaller than the wavelength and is therefore largely
justified for the long terrestrial wavelengths but might be inaccurate in the presence of super coarse particles <xref ref-type="bibr" rid="bib1.bibx13" id="paren.31"/>.  However,
this only affects the direct radiative effect. In the context of the present
study, the indirect radiative effect turns out to be much more relevant.</p>
      <p id="d1e941">Aerosol removal by wet deposition is calculated by the scavenging submodel SCAV
<xref ref-type="bibr" rid="bib1.bibx58" id="paren.32"/>, dry deposition and sedimentation by the submodels DDEP
and SEDI <xref ref-type="bibr" rid="bib1.bibx24" id="paren.33"/>.  The aerosol and in particular the mineral
dust representation in EMAC have a proven track record
<xref ref-type="bibr" rid="bib1.bibx1 bib1.bibx2 bib1.bibx46 bib1.bibx30 bib1.bibx7 bib1.bibx47 bib1.bibx44" id="paren.34"><named-content content-type="pre">e.g.</named-content></xref>: the dust aerosol optical depth is consistent with observations not only at visible
wavelengths, but also in the infrared at 10 <inline-formula><mml:math id="M55" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m <xref ref-type="bibr" rid="bib1.bibx30" id="paren.35"/>.  This is an indication of a realistic particle size distribution, provided that the ratio
of the extinction efficiencies at visible and infrared wavelengths is realistic.
The uncertainty in this ratio is expected to be small compared to other
uncertainties, given that the spectral extinction efficiency is calculated
consistently throughout the spectrum and, unlike the single scattering albedo,
is hardly sensitive to the aforementioned uncertainties in the imaginary part of
the refractive index.</p>
      <p id="d1e967">Large-scale clouds are simulated by the submodel CLOUD <xref ref-type="bibr" rid="bib1.bibx19" id="paren.36"/>, where different parametrisations of cloud droplet formation and ice nucleation
are implemented. We use a two-moment stratiform cloud microphysics scheme
<xref ref-type="bibr" rid="bib1.bibx42 bib1.bibx43 bib1.bibx40" id="paren.37"/> in
combination with the UAF (Unified Activation Framework) cloud droplet activation
parametrisation <xref ref-type="bibr" rid="bib1.bibx32 bib1.bibx20 bib1.bibx22" id="paren.38"/>.
For the ice crystal formation we use the comprehensive parametrisation for
cirrus and mixed-phase clouds implemented by <xref ref-type="bibr" rid="bib1.bibx5" id="text.39"/> based on
<xref ref-type="bibr" rid="bib1.bibx6" id="text.40"/>.  Convective clouds are calculated by the CONVECT
submodel <xref ref-type="bibr" rid="bib1.bibx19" id="paren.41"/>, where interactions with aerosols are not taken
into account. CONVECT provides a choice of convection schemes
<xref ref-type="bibr" rid="bib1.bibx59" id="paren.42"/>, and here we use the scheme of <xref ref-type="bibr" rid="bib1.bibx57" id="text.43"/> including
modifications by <xref ref-type="bibr" rid="bib1.bibx50" id="text.44"/>.  The optical properties of clouds which serve as
input for the radiative transfer submodel RAD are computed by the submodel
CLOUDOPT <xref ref-type="bibr" rid="bib1.bibx14" id="paren.45"/>.  The model yields a global annual mean cloud
liquid water path around 80 g<inline-formula><mml:math id="M56" display="inline"><mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> (Tables <xref ref-type="table" rid="Ch1.T1"/> and S3 in the Supplement), which is well within the range of other climate
model results <xref ref-type="bibr" rid="bib1.bibx34" id="paren.46"><named-content content-type="pre">32 to 125 g<inline-formula><mml:math id="M57" display="inline"><mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>,</named-content></xref> and
observations <xref ref-type="bibr" rid="bib1.bibx41" id="paren.47"><named-content content-type="pre">30 to
90 g<inline-formula><mml:math id="M58" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>,</named-content></xref>.  Likewise, the
modelled annual mean global cloud ice water path of about
15 g<inline-formula><mml:math id="M59" display="inline"><mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> (Tables <xref ref-type="table" rid="Ch1.T1"/> and S3 in the
Supplement) is consistent with results from other models <xref ref-type="bibr" rid="bib1.bibx41" id="paren.48"><named-content content-type="pre">e.g. 14.8 g<inline-formula><mml:math id="M60" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>,</named-content></xref> and close to observed values <xref ref-type="bibr" rid="bib1.bibx39" id="paren.49"><named-content content-type="pre">e.g. (25 <inline-formula><mml:math id="M61" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 7) g<inline-formula><mml:math id="M62" display="inline"><mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>,</named-content></xref>.</p>

<table-wrap id="Ch1.T2" specific-use="star"><?xmltex \currentcnt{2}?><label>Table 2</label><caption><p id="d1e1126">Globally averaged annual mean TOA ERFs in W m<inline-formula><mml:math id="M63" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, based on the SST
simulations. “Mineral dust” and “Anthropogenic pollution” include the
effect of dust–pollution interactions (<inline-formula><mml:math id="M64" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>x</mml:mi></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M65" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">pol</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>x</mml:mi></mml:mrow></mml:math></inline-formula> in
Eq. <xref ref-type="disp-formula" rid="Ch1.E1"/>); “Dust–pollution interactions” are given by the  interaction term <inline-formula><mml:math id="M66" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>x</mml:mi></mml:mrow></mml:math></inline-formula>, Eq. (<xref ref-type="disp-formula" rid="Ch1.E2"/>).  The  corresponding forcings obtained from the nudged simulations are provided in
Table S4 in the Supplement.</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="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">Mineral dust</oasis:entry>
         <oasis:entry colname="col4">Anthropogenic pollution</oasis:entry>
         <oasis:entry colname="col5">Dust–pollution interactions</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Total</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M67" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.01 <inline-formula><mml:math id="M68" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.07</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M69" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.6 <inline-formula><mml:math id="M70" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1</oasis:entry>
         <oasis:entry colname="col5">0.2 <inline-formula><mml:math id="M71" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Net</oasis:entry>
         <oasis:entry colname="col2">Direct</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M72" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.260 <inline-formula><mml:math id="M73" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.006</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M74" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.490 <inline-formula><mml:math id="M75" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.005</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M76" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.054 <inline-formula><mml:math id="M77" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.005</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Indirect</oasis:entry>
         <oasis:entry colname="col3">0.25 <inline-formula><mml:math id="M78" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.07</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M79" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.1 <inline-formula><mml:math id="M80" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1</oasis:entry>
         <oasis:entry colname="col5">0.3 <inline-formula><mml:math id="M81" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Total</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M82" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.04 <inline-formula><mml:math id="M83" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.06</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M84" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.86 <inline-formula><mml:math id="M85" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.06</oasis:entry>
         <oasis:entry colname="col5">0.3 <inline-formula><mml:math id="M86" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">SW</oasis:entry>
         <oasis:entry colname="col2">Direct</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M87" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.367 <inline-formula><mml:math id="M88" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.007</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M89" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.527 <inline-formula><mml:math id="M90" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.005</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M91" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.058 <inline-formula><mml:math id="M92" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.005</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Indirect</oasis:entry>
         <oasis:entry colname="col3">0.33 <inline-formula><mml:math id="M93" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.07</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M94" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.33 <inline-formula><mml:math id="M95" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.06</oasis:entry>
         <oasis:entry colname="col5">0.3 <inline-formula><mml:math id="M96" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Total</oasis:entry>
         <oasis:entry colname="col3">0.03 <inline-formula><mml:math id="M97" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08</oasis:entry>
         <oasis:entry colname="col4">0.26 <inline-formula><mml:math id="M98" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.07</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M99" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.07 <inline-formula><mml:math id="M100" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">LW</oasis:entry>
         <oasis:entry colname="col2">Direct</oasis:entry>
         <oasis:entry colname="col3">0.107 <inline-formula><mml:math id="M101" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.001</oasis:entry>
         <oasis:entry colname="col4">0.0368 <inline-formula><mml:math id="M102" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.0009</oasis:entry>
         <oasis:entry colname="col5">0.004 <inline-formula><mml:math id="M103" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.001</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Indirect</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M104" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.08 <inline-formula><mml:math id="M105" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08</oasis:entry>
         <oasis:entry colname="col4">0.22 <inline-formula><mml:math id="M106" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.07</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M107" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.08 <inline-formula><mml:math id="M108" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d1e1677">A complete list of the MESSy submodels used in our simulations is provided in
Table S2 in the Supplement.  Descriptions of each submodel and further
references can be found online in the MESSy submodel list <xref ref-type="bibr" rid="bib1.bibx45" id="paren.50"/>.</p>
</sec>
<?pagebreak page15288?><sec id="Ch1.S3">
  <label>3</label><title>Methodology</title>
      <p id="d1e1691">We apply a similar analysis to <xref ref-type="bibr" rid="bib1.bibx31" id="text.51"/>, which is based on simulations with four different emission set-ups: a baseline simulation with
neither dust nor anthropogenic emissions (“0”), a simulation with dust but
without anthropogenic emissions (“dust”), a simulation with anthropogenic
pollution but without dust emissions (“pol”) and a full simulation considering
all emissions.</p>
      <p id="d1e1697">In the anthropogenic pollution-free simulations (“0”, “dust”) we disable the EDGAR emissions including <inline-formula><mml:math id="M109" display="inline"><mml:mrow><mml:msub><mml:mtext>SO</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M110" display="inline"><mml:mrow><mml:msub><mml:mtext>NH</mml:mtext><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M111" display="inline"><mml:mrow><mml:msub><mml:mtext>NO</mml:mtext><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, and black and organic carbon emissions but retain the greenhouse gases. We attribute
90 % of the GFED biomass burning emissions to human activities
<xref ref-type="bibr" rid="bib1.bibx38" id="paren.52"/> and reduce them accordingly, whereas we do not consider
anthropogenic factors in dust emissions such as land use and climate change <xref ref-type="bibr" rid="bib1.bibx29" id="paren.53"/>, assuming all dust emissions to be natural.</p>
      <p id="d1e1739">A result <inline-formula><mml:math id="M112" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> from the full simulation (e.g. the annual global mean cloud liquid water content) is related to the corresponding result from the baseline
simulation <inline-formula><mml:math id="M113" display="inline"><mml:mrow><mml:msub><mml:mi>x</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> by
          <disp-formula id="Ch1.E1" content-type="numbered"><label>1</label><mml:math id="M114" display="block"><mml:mrow><mml:mi>x</mml:mi><mml:mo>=</mml:mo><mml:msub><mml:mi>x</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">pol</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
        where <inline-formula><mml:math id="M115" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>=</mml:mo><mml:msub><mml:mi>x</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>x</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M116" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">pol</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>=</mml:mo><mml:msub><mml:mi>x</mml:mi><mml:mi mathvariant="normal">pol</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>x</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and
          <disp-formula id="Ch1.E2" content-type="numbered"><label>2</label><mml:math id="M117" display="block"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>x</mml:mi><mml:mo>=</mml:mo><mml:mi>x</mml:mi><mml:mo>-</mml:mo><mml:msub><mml:mi>x</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>x</mml:mi><mml:mi mathvariant="normal">pol</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi>x</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
        which represents the effect of the dust–pollution interactions. In the absence of such interactions, the term <inline-formula><mml:math id="M118" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>x</mml:mi></mml:mrow></mml:math></inline-formula> vanishes.  We apply
Eq. (<xref ref-type="disp-formula" rid="Ch1.E2"/>) to the annual mean cloud liquid and ice water paths and radiative fluxes.</p>
      <p id="d1e1915">To quantify the effects of the different emission set-ups and the dust–pollution interactions on radiation, we consider the ERF, which is defined as the change in net TOA downward radiative flux after allowing
for atmospheric temperatures, water vapour and clouds to adjust but with sea surface temperature (SST) and sea ice cover fixed at climatological values <xref ref-type="bibr" rid="bib1.bibx18" id="paren.54"/>. Note that positive downward fluxes correspond to downward
(incoming) radiation; negative values correspond to upward (outgoing) radiation. The ERF accounts for rapid adjustments by radiative and dynamical feedbacks,
whereas it excludes long-term climate responses involving the much slower
thermal equilibration of the oceans.  Due to the limited constraints on the
atmospheric dynamics in SST simulations, the meteorological variability is large, and hence a sufficient number of years has to be simulated to obtain
statistically significant results.  We perform SST simulations long enough to
yield significant globally averaged results; however, detailed regional analysis would require much longer SST simulations.  In order to nevertheless gain
insights from regional evaluation, we additionally use simulations where the
model dynamics above the boundary layer is nudged to meteorological analyses of
the European Centre for Medium-Range Weather Forecasts<?pagebreak page15289?> (ECMWF). Within the
boundary layer, in the topmost layers and to some extent in between, nudged quantities like the temperature may still respond to other variables such as
radiative fluxes (soft nudging). The nudging greatly reduces the influence of
inter-annual variability on statistical analysis. The results from the nudged
simulations turn out to be largely consistent with those of the SST simulations
(Tables <xref ref-type="table" rid="Ch1.T1"/>, <xref ref-type="table" rid="Ch1.T2"/> vs. S3, S4 in the
Supplement); in particular, the estimates for the total global radiative effect of the dust–pollution interactions agree within the error bounds, so that the use of nudged simulations for the regional analysis is reasonable and helpful.</p>
      <p id="d1e1926">With prescribed SST we run ensembles of 16
simulations, each covering 1 year.  As there is one ensemble for each of the four emission set-ups, in total this amounts to 64 SST simulations.  The ensemble members are obtained by
perturbing temperature and humidity in the fourth year of a common spin-up
simulation, followed by an additional spin-up of the individual ensemble members
to attain a total of 5 spin-up years.  The perturbation is implemented by adding
a uniformly distributed random variable ranging from <inline-formula><mml:math id="M119" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>0.1 ‰ to
0.1 ‰ of the perturbed quantity, so that the perturbation is numerically but not meteorologically relevant.  Emission data for 2010 are used for all simulations.  The nudged simulations cover 10 years from 2006 to 2015, and 2 simulation years prior to that period were used for the model spin-up.  To
estimate the uncertainties of the 10-year mean values for the nudged simulations
and the ensemble mean values for the SST simulations, we compute the standard
error of the mean (SEM) of the annual values.</p>
      <p id="d1e1936">In the analysis of the SST results, we substitute the variable <inline-formula><mml:math id="M120" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> in
Eq. (<xref ref-type="disp-formula" rid="Ch1.E2"/>) with global annual mean values, and for the nudged
results we skip the global averaging and apply the equation to the annual mean
for each grid cell separately to obtain the spatial distribution of the
interaction term.</p>
      <p id="d1e1948">Substituting <inline-formula><mml:math id="M121" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> for the global annual mean net flux <inline-formula><mml:math id="M122" display="inline"><mml:mi>F</mml:mi></mml:math></inline-formula> at the top of the atmosphere (TOA) in the SST simulations, <inline-formula><mml:math id="M123" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub><mml:mi>F</mml:mi><mml:mo>=</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> corresponds to the total ERF of mineral dust including
all rapid adjustments, analogous to <inline-formula><mml:math id="M124" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">pol</mml:mi></mml:msub><mml:mi>F</mml:mi></mml:mrow></mml:math></inline-formula> to the anthropogenic aerosol ERF (both excluding the dust–pollution interactions) and <inline-formula><mml:math id="M125" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>F</mml:mi></mml:mrow></mml:math></inline-formula> to the ERF of dust–pollution interactions.  In the case of
the nudged simulations, the possible adjustments are constrained, so that the resulting forcings are in between the ERF and the radiative forcing RF as
defined by <xref ref-type="bibr" rid="bib1.bibx18" id="text.55"/>, where only the stratospheric temperature is allowed to adjust. For this reason the forcings from the nudged simulations are
not directly comparable to RF and ERF results but, as mentioned above, provide valuable information about the regional effects.</p>
      <p id="d1e2022">To compute the direct radiative effect of aerosols, the radiative transfer code
is called twice for every model time step. The first call considers scattering
and absorption by aerosols and is used to calculate the heating rates affecting
the temperature; the second call ignores scattering and absorption by aerosols and computes the radiative fluxes and heating rates only for diagnostic output.
The difference of the radiative fluxes from both calls yields the instantaneous
forcing (IRF) due to the direct radiative effect of aerosols <inline-formula><mml:math id="M126" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">ari</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>.
Since both calls are performed with identical clouds, the cloud forcing is
excluded, and only little statistical noise is introduced by the strong variability of clouds.  Nevertheless, in this way we obtain the direct radiative
forcing in the presence of clouds, which is typically smaller than the clear-sky forcing.  The difference of the instantaneous aerosol forcings in the SST
simulations with and without mineral dust <inline-formula><mml:math id="M127" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">ari</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mrow><mml:mi mathvariant="normal">ari</mml:mi><mml:mo>,</mml:mo><mml:mi mathvariant="normal">dust</mml:mi></mml:mrow></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mrow><mml:mi mathvariant="normal">ari</mml:mi><mml:mo>,</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> yields the aerosol–radiation interaction contribution to the ERF of dust, i.e. the direct radiative effect of dust. Analogously <inline-formula><mml:math id="M128" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">pol</mml:mi></mml:msub><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">ari</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and
<inline-formula><mml:math id="M129" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">ari</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> represent the direct radiative effect of
particulate pollution and the dust–pollution interactions.  The direct radiative forcings are subtracted from the corresponding total aerosol radiative forcings
to extract the indirect radiative forcings; e.g. the indirect contribution to the dust–pollution interaction forcing is <inline-formula><mml:math id="M130" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>F</mml:mi><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">ari</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><?xmltex \currentcnt{1}?><label>Figure 1</label><caption><p id="d1e2135">Annual mean effect of the dust–pollution interactions on the liquid <bold>(a)</bold> and ice <bold>(b)</bold> cloud water, calculated by applying Eq. (<xref ref-type="disp-formula" rid="Ch1.E2"/>) to  the results of the nudged simulations. Over stippled regions the results
differ from zero by less than 2 times the standard error of the mean (SEM) of the annual values.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/20/15285/2020/acp-20-15285-2020-f01.png"/>

      </fig>

<?xmltex \hack{\newpage}?>
</sec>
<?pagebreak page15290?><sec id="Ch1.S4">
  <label>4</label><title>Effects on the cloud condensate</title>
      <p id="d1e2162">Hydrophilic particulate anthropogenic pollution enhances the cloud droplet
formation and thus the liquid water content (Table <xref ref-type="table" rid="Ch1.T1"/>).
However, in the presence of mineral dust particles this effect is reduced
because fine pollution particles coagulate with coarse dust particles, decreasing the particle number and virtually cleaning the atmosphere of fine particulate
pollution.  Moreover, the adsorption activation of mineral dust particles occurs
early on in the cloud formation process <xref ref-type="bibr" rid="bib1.bibx32" id="paren.56"/>, reducing the
maximum supersaturation and inhibiting the activation of small pollution
particles. These effects reduce the number of cloud condensation nuclei
<xref ref-type="bibr" rid="bib1.bibx20 bib1.bibx22" id="paren.57"/> and decrease the cloud liquid water
path as shown in Fig. <xref ref-type="fig" rid="Ch1.F1"/>a. Especially over East and South
Asia, where strong pollution emissions mix with aeolian dust from the
Taklamakan, Gobi and Thar deserts, the reduction is substantial and regionally
exceeds <inline-formula><mml:math id="M131" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>40 g<inline-formula><mml:math id="M132" display="inline"><mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. Even over polluted regions in Europe and the
USA which are only occasionally exposed to dust intrusions, we obtain a small
but significant reduction.  This negative impact of the dust–pollution interactions over large parts of the Northern Hemisphere leads to a reduction of
the global mean cloud liquid water path in Fig. <xref ref-type="fig" rid="Ch1.F1"/>a by
(<inline-formula><mml:math id="M133" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>1.10 <inline-formula><mml:math id="M134" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03) g<inline-formula><mml:math id="M135" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>.  A comparable reduction
by (<inline-formula><mml:math id="M136" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>1.5 <inline-formula><mml:math id="M137" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.2) g<inline-formula><mml:math id="M138" display="inline"><mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> is obtained in the SST
simulations (Table <xref ref-type="table" rid="Ch1.T1"/>).  Relative to the mean liquid water path
in the SST simulation considering all emissions
(85.5 <inline-formula><mml:math id="M139" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1) g<inline-formula><mml:math id="M140" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, these reductions appear to be rather moderate.
The reason is that the transport time periods between most of the major dust
sources, especially the Sahara and the Middle East, and major pollution sources
like North America and Europe to a large degree exceed the dust aerosol lifetime.  In Asia these sources are less distant, while pollution emissions are
generally larger. Thus, the strong effects over Asia might provide an outlook
for regions with emerging pollution sources close to dust sources in Africa and
the Middle East. But already today, due to the critical influence of clouds on
radiative transfer, the relatively small changes in the water paths cause substantial radiative forcings, as will be discussed in the next section.</p>
      <p id="d1e2283">The dust–pollution interaction effect on the cloud ice water path, shown in Fig. <xref ref-type="fig" rid="Ch1.F1"/>b, is less distinct.  A negative impact is obtained
over the Sahel. The direct radiative effect of mineral dust over the Sahara
warms the atmosphere by absorption of solar radiation (Fig. S1a in the
Supplement). This increases the atmospheric capacity to hold moisture and the
vertical water vapour transport (Fig. S1b in the Supplement).  As a result,
more moisture is available for ice cloud formation (Fig. S1c in the
Supplement). Since the net direct radiative effect of the dust–pollution interactions cools the atmosphere over the Sahara <xref ref-type="bibr" rid="bib1.bibx31" id="paren.58"/>, it
moderates the enhancement of ice cloud formation.  A similar net cooling effect
is found over the region around the Taklamakan and Gobi deserts.  In this region
with generally high ice water content, anthropogenic pollution enhances the ice
water path, but adding dust reduces the number of anthropogenic ice nucleation
particles via coagulation.  In contrast, a positive impact is obtained over
coastal regions of Canada and Greenland around 60<inline-formula><mml:math id="M141" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, probably due to
aerosol and cloud feedbacks on the polar and Ferrel cell circulations and
associated vertical moisture transport. However, because of the comparably small
radiative fluxes at these latitudes, this has relatively little impact on
radiative fluxes from a global perspective.  Due to the regionally varying sign
of the dust–pollution interaction effect on cloud ice, the global mean in Fig. <xref ref-type="fig" rid="Ch1.F1"/>b is close to zero,
(<inline-formula><mml:math id="M142" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.027 <inline-formula><mml:math id="M143" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.003) g<inline-formula><mml:math id="M144" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. The corresponding value
in the SST simulations, (<inline-formula><mml:math id="M145" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.02 <inline-formula><mml:math id="M146" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03) g<inline-formula><mml:math id="M147" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, is consistent with this
result, being several orders of magnitude smaller than the global mean ice water
path in the SST simulation considering all emissions,
(14.70 <inline-formula><mml:math id="M148" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01) g<inline-formula><mml:math id="M149" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>
(Table <xref ref-type="table" rid="Ch1.T1"/>).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><?xmltex \currentcnt{2}?><label>Figure 2</label><caption><p id="d1e2388">Annual mean indirect effect of the dust–pollution interactions on the  solar <bold>(a)</bold> and terrestrial <bold>(b)</bold> radiative forcing at the top of the atmosphere,
calculated by applying Eq. (<xref ref-type="disp-formula" rid="Ch1.E2"/>) to the results of the nudged
simulations. Over stippled regions the results differ from zero by less than
2 times the SEM of the annual values.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/20/15285/2020/acp-20-15285-2020-f02.png"/>

      </fig>

<?xmltex \hack{\newpage}?>
</sec>
<?pagebreak page15291?><sec id="Ch1.S5">
  <label>5</label><title>Radiative effects</title>
      <p id="d1e2416">The reduction of the cloud water content by dust–pollution interactions has a significant impact on the transfer of solar radiation (“shortwave”, SW), which
is shown in Fig. <xref ref-type="fig" rid="Ch1.F2"/>a. With reduced
liquid cloud water, less solar radiation is reflected back to space; i.e. the outgoing radiation and the associated negative contribution to the net flux decrease, corresponding to a net positive forcing at the TOA. Comparing
Figs. <xref ref-type="fig" rid="Ch1.F2"/>a and <xref ref-type="fig" rid="Ch1.F1"/>a reveals the one-to-one correspondence of the
dust–pollution interaction effect on the liquid cloud water and solar radiation. Over the polluted regions of the Northern Hemisphere, i.e. Asia, Europe and North America, and over the Atlantic Ocean along the northern African coast in the
Saharan dust outflow, the positive forcing can exceed 2 W m<inline-formula><mml:math id="M150" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>.
Globally averaged, the net forcing in the solar spectrum shown in
Fig. <xref ref-type="fig" rid="Ch1.F2"/>a is
(0.23 <inline-formula><mml:math id="M151" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01) W m<inline-formula><mml:math id="M152" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, and the SST simulations yield an ERF of (0.3 <inline-formula><mml:math id="M153" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1) W m<inline-formula><mml:math id="M154" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
(Table <xref ref-type="table" rid="Ch1.T2"/>).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><?xmltex \currentcnt{3}?><label>Figure 3</label><caption><p id="d1e2482">Total (direct and indirect, SW and LW) annual mean effect of the
dust–pollution interactions on the radiative forcing at the top of the  atmosphere, calculated by applying Eq. (<xref ref-type="disp-formula" rid="Ch1.E2"/>) to the results of
the nudged simulations. Over stippled regions the results differ from zero by
less than 2 times the SEM of the annual values.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/20/15285/2020/acp-20-15285-2020-f03.png"/>

      </fig>

      <p id="d1e2493">On the other hand, the dust–pollution interaction effect on the terrestrial spectrum (“longwave”, LW), Fig. <xref ref-type="fig" rid="Ch1.F2"/>b,
is directly related to the effects on ice clouds,
Fig. <xref ref-type="fig" rid="Ch1.F1"/>b. This is most distinct over the Sahel but also apparent over the East Asian deserts. The reduced cloud ice water path over
these regions traps less outgoing terrestrial radiation, resulting in a net cooling from the dust–pollution interactions. Over the Sahel the terrestrial TOA forcing reaches <inline-formula><mml:math id="M155" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>2 W m<inline-formula><mml:math id="M156" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>.  With regard to the radiative energy
budget, the regions with a significant dust–pollution interaction effect on cloud ice in Fig. <xref ref-type="fig" rid="Ch1.F1"/>b are of different relevance. The
Sahel, where the dust–pollution interactions reduce cloud ice, is relatively close to the Equator, and accordingly stronger radiative fluxes are affected by
the cloud ice changes than in the other regions, hence the global net radiative
effect related to cloud ice is more relevant than the global net effect on cloud
ice itself.  Globally averaged, the net forcing in the terrestrial spectrum
shown in Fig. <xref ref-type="fig" rid="Ch1.F2"/>b is
(<inline-formula><mml:math id="M157" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.05 <inline-formula><mml:math id="M158" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01) W m<inline-formula><mml:math id="M159" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, and the SST simulations
yield an ERF of (<inline-formula><mml:math id="M160" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.08 <inline-formula><mml:math id="M161" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09) W m<inline-formula><mml:math id="M162" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
(Table <xref ref-type="table" rid="Ch1.T2"/>).</p>
      <p id="d1e2580">Thus, a substantial positive forcing in the solar spectrum is partially
compensated by a negative forcing in the terrestrial spectrum to yield a still
considerable, positive net forcing associated with the effect of dust–pollution interactions on clouds. The global distribution of the total net forcing at the TOA including the direct radiative effect is shown in
Fig. <xref ref-type="fig" rid="Ch1.F3"/>. The regional forcing ranges from below
<inline-formula><mml:math id="M163" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>2 W m<inline-formula><mml:math id="M164" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> over the Sahel to above 2 W m<inline-formula><mml:math id="M165" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> over Asia.
Even though overall these contributions partially counterbalance, at (0.15 <inline-formula><mml:math id="M166" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02) W m<inline-formula><mml:math id="M167" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> the corresponding global
mean forcing in Fig. <xref ref-type="fig" rid="Ch1.F3"/> is significantly
positive. Consistently, the ERF in the SST simulations is
(0.2 <inline-formula><mml:math id="M168" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1) W m<inline-formula><mml:math id="M169" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
(Table <xref ref-type="table" rid="Ch1.T2"/>).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><?xmltex \currentcnt{4}?><label>Figure 4</label><caption><p id="d1e2661">Estimates of the global anthropogenic aerosol forcings at the top of
the atmosphere (TOA) in the presence (“With dust”, <inline-formula><mml:math id="M170" display="inline"><mml:mrow><mml:mi>F</mml:mi><mml:mo>-</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">dust</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) or  absence (“Without dust”, <inline-formula><mml:math id="M171" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">pol</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) of aeolian dust,  based on the SST simulations.  The total forcings comprise the direct (green,
<inline-formula><mml:math id="M172" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">ari</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mrow><mml:mi mathvariant="normal">ari</mml:mi><mml:mo>,</mml:mo><mml:mi mathvariant="normal">dust</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M173" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mrow><mml:mi mathvariant="normal">ari</mml:mi><mml:mo>,</mml:mo><mml:mi mathvariant="normal">pol</mml:mi></mml:mrow></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>F</mml:mi><mml:mrow><mml:mi mathvariant="normal">ari</mml:mi><mml:mo>,</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula>) and indirect (blue) forcings. The change caused by
including mineral dust corresponds to the positive forcing of dust–pollution  interactions <inline-formula><mml:math id="M174" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi mathvariant="normal">int</mml:mi></mml:msub><mml:mi>F</mml:mi></mml:mrow></mml:math></inline-formula> (red).  Darker colours represent the
SEM.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/20/15285/2020/acp-20-15285-2020-f04.png"/>

      </fig>

      <p id="d1e2767">Figure <xref ref-type="fig" rid="Ch1.F4"/> summarises the direct and indirect global TOA ERF
of anthropogenic aerosol interacting with mineral dust and in the absence of
mineral dust, obtained from the SST simulations. Despite the more negative
anthropogenic aerosol direct radiative forcing in the presence of mineral dust,
already reported by <xref ref-type="bibr" rid="bib1.bibx31" id="text.59"/>, the effect of mineral dust on the
total forcing is clearly dominated by the moderation of the indirect forcing.
The figure highlights the importance of the dust–pollution interactions for assessing the cooling effect of anthropogenic aerosol: the cooling is
substantially reduced by the interactions from (<inline-formula><mml:math id="M175" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.81 <inline-formula><mml:math id="M176" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.06) W m<inline-formula><mml:math id="M177" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
ERF, which is close to 0.9 W m<inline-formula><mml:math id="M178" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> estimated by <xref ref-type="bibr" rid="bib1.bibx18" id="text.60"/>,
down to (<inline-formula><mml:math id="M179" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>0.6 <inline-formula><mml:math id="M180" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1) W m<inline-formula><mml:math id="M181" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>.</p><?xmltex \hack{\newpage}?>
</sec>
<?pagebreak page15292?><sec id="Ch1.S6" sec-type="conclusions">
  <label>6</label><title>Conclusions</title>
      <p id="d1e2852">We have studied the effects of interactions between mineral dust and
anthropogenic pollution on clouds and radiation by analysing comprehensive
global simulations performed with the atmospheric chemistry-climate model EMAC.
Four different emission configurations representing all possible combinations of
including and excluding dust and pollution were considered. Comparing the results for these four scenarios allowed us to isolate the effect of the dust–pollution
interactions from the individual effects of dust and pollution.  Several aspects
make this analysis challenging, should be considered when interpreting the results, and may leave room for refinements in future studies.  Naturally,
clouds are subject to strong variability; hence, although we performed ensemble simulations, there is considerable statistical uncertainty in the present
results. This adds to the need to evaluate differences in differences of results
from a number of simulations to obtain the interaction effect, which increases
the relative error. Moreover, a wide range of physical and chemical processes is
involved in the dust–pollution interactions, and accordingly many submodels and parametrisations within EMAC contribute to our final result and uncertainty.
Even though the parametrisations are well established and tested, the analysis
might be sensitive to systematic errors of some of them.</p>
      <p id="d1e2855">The analysis reveals that the cloud water path is reduced by the dust–pollution interactions as they moderate the cloud water path increase caused by
anthropogenic pollution.  The reason for this moderation is that mineral dust
particles decrease the number of anthropogenic cloud condensation nuclei by
coagulation and additionally limit the activation of the fine hydrophilic
anthropogenic particles by lowering the maximum supersaturation through
adsorption activation.  Dust–pollution interaction effects on the cloud ice content are noticeable as well but less relevant.</p>
      <p id="d1e2858">The atmospheric radiative transfer is very sensitive to the reduction of the
cloud water path.  Generally, dust–pollution interactions affect the radiative transfer at all wavelengths (solar and terrestrial) by modifying both the direct
aerosol–radiation interactions and the indirect radiative effect of aerosols via cloud adjustments.  However, the total radiative effect of the dust–pollution
interactions is dominated by the impact through the indirect effect which, in
contrast to the direct effect, exerts an overall positive TOA net forcing.  The impact on the indirect radiative effect in turn is dominated by that on solar
radiation fluxes. In this case, the aforementioned decrease in the cloud water path reduces the cloud albedo and the reflection of solar radiation, resulting
in a positive contribution to the radiative net flux.</p>
      <p id="d1e2861">We estimate that dust–pollution interactions contribute (0.2 <inline-formula><mml:math id="M182" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1) W m<inline-formula><mml:math id="M183" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> to the global mean
anthropogenic aerosol effective radiative forcing, significantly reducing the
climate cooling effect of atmospheric aerosols.  In view of this considerable
contribution to the atmospheric energy balance, it is recommended to account for
the dust–pollution interactions in assessments of climate change, especially because on a regional scale effects can be even larger. The net global effect
partially depends on regionally counteracting positive and negative radiative
forcings. This study emphasises the importance of continued efforts to improve the understanding and parametrisations of the processes involved in order to
reduce the uncertainty of future climate simulations.</p>
</sec>

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

      <p id="d1e2887">The Modular Earth Submodel System (MESSy) is continuously further developed
and applied by a consortium of institutions. The usage of MESSy and access to
the source code are licensed to all affiliates of institutions which are  members of the MESSy Consortium. Institutions can become a member of the MESSy
Consortium by signing the MESSy Memorandum of Understanding. More information
can be found on the MESSy Consortium website  (<uri>https://www.messy-interface.org</uri>, last
access: 30 October 2020, <xref ref-type="bibr" rid="bib1.bibx45" id="altparen.61"/>).  The ECHAM climate model is available to the
scientific community under the MPI-M Software License Agreement
(<uri>https://mpimet.mpg.de/en/science/modeling-with-icon/code-availability</uri>,  last access: 30 October 2020, <xref ref-type="bibr" rid="bib1.bibx49" id="altparen.62"/>).  The simulation results analysed in this study
are available at  <uri>https://edmond.mpdl.mpg.de/imeji/collection/V5fqhlhJgMJAJ3</uri> (last
access: 30 October 2020, <xref ref-type="bibr" rid="bib1.bibx27" id="altparen.63"/>).</p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d1e2909">The supplement related to this article is available online at: <inline-supplementary-material xlink:href="https://doi.org/10.5194/acp-20-15285-2020-supplement" xlink:title="pdf">https://doi.org/10.5194/acp-20-15285-2020-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e2918">KK performed the simulations assisted by VAK and SB, analysed the model results
and wrote the article supported by JL, SB, VAK and GLS. All the authors discussed the results and contributed to the final manuscript.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e2924">The authors declare that they have no conflict of interest.</p>
  </notes><notes notes-type="sistatement"><title>Special issue statement</title>

      <p id="d1e2930">This article is part of the special issue “The Modular Earth Submodel System (MESSy) (ACP/GMD inter-journal SI)”. It is not associated with a conference.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e2936">The research reported in this publication has received funding from the MaxWater initiative of the Max Planck Society and the King Abdullah University of Science and Technology project “Combined Radiative and Air Quality Effects of Anthropogenic Air Pollution and Dust over the Arabian Peninsula”.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <?pagebreak page15293?><p id="d1e2941">This research has been supported by the King Abdullah University of Science and Technology (grant CRG3, grant no. URF/1/2180-01-01).<?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.</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e2953">This paper was edited by Yves Balkanski and reviewed by two anonymous referees.</p>
  </notes><ref-list>
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<abstract-html><p>The interactions between aeolian dust and anthropogenic air pollution, notably  chemical ageing of mineral dust and coagulation of dust and pollution
particles, modify the atmospheric aerosol composition and burden. Since the
aerosol particles can act as cloud condensation nuclei, this affects  the radiative transfer not only directly via aerosol–radiation interactions, but also  indirectly through cloud adjustments. We study both radiative effects using
the global ECHAM/MESSy atmospheric chemistry-climate model (EMAC) which
combines the Modular Earth Submodel System (MESSy) with the European
Centre/Hamburg (ECHAM) climate model. Our simulations show that
dust–pollution–cloud interactions reduce the condensed water path and hence  the reflection of solar radiation. The associated climate warming outweighs
the cooling that the dust–pollution interactions exert through the direct  radiative effect. In total, this results in a net warming by dust–pollution
interactions which moderates the negative global anthropogenic aerosol forcing
at the top of the atmosphere by (0.2&thinsp;±&thinsp;0.1) W&thinsp;m<sup>−2</sup>.</p></abstract-html>
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