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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-18-17225-2018</article-id><title-group><article-title>Coarse-mode mineral dust size distributions, composition and optical
properties from AER-D aircraft measurements <?xmltex \hack{\break}?>over the tropical eastern
Atlantic</article-title><alt-title>Coarse-mode mineral dust size distributions</alt-title>
      </title-group><?xmltex \runningtitle{Coarse-mode mineral dust size distributions}?><?xmltex \runningauthor{C. L. Ryder et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Ryder</surname><given-names>Claire L.</given-names></name>
          <email>c.l.ryder@reading.ac.uk</email>
        <ext-link>https://orcid.org/0000-0002-9892-6113</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Marenco</surname><given-names>Franco</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1833-1102</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Brooke</surname><given-names>Jennifer K.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-5752-5877</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Estelles</surname><given-names>Victor</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Cotton</surname><given-names>Richard</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Formenti</surname><given-names>Paola</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-0372-1351</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>McQuaid</surname><given-names>James B.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-8702-0415</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff6">
          <name><surname>Price</surname><given-names>Hannah C.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Liu</surname><given-names>Dantong</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-3768-1770</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Ausset</surname><given-names>Patrick</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5 aff8">
          <name><surname>Rosenberg</surname><given-names>Phil D.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-6920-0559</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Taylor</surname><given-names>Jonathan W.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-2120-186X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Choularton</surname><given-names>Tom</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-0409-4329</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Bower</surname><given-names>Keith</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-9802-3264</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Coe</surname><given-names>Hugh</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-3264-1713</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Gallagher</surname><given-names>Martin</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-4968-6088</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7 aff9">
          <name><surname>Crosier</surname><given-names>Jonathan</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-3086-4729</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Lloyd</surname><given-names>Gary</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Highwood</surname><given-names>Eleanor J.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>Murray</surname><given-names>Benjamin J.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-8198-8131</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Department of Meteorology, University of Reading, Reading, RG6 6BB, UK</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Met Office, Exeter, UK</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Department de Física de la Terra i Termodinàmica, Universitat de
València, 46100 Burjassot, Spain</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>LISA, UMR CNRS 7583/Université Paris Est Créteil et Université
Paris Diderot, Institut Pierre Simon<?xmltex \hack{\break}?> Laplace, Créteil, France</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>School of Earth and Environment, University of Leeds, Woodhouse Lane, Leeds, LS2
9JT, UK</institution>
        </aff>
        <aff id="aff6"><label>6</label><institution>Facility for Atmospheric Airborne Measurements, Cranfield, UK</institution>
        </aff>
        <aff id="aff7"><label>7</label><institution>Centre for Atmospheric Sciences, School of Earth and Environmental
Sciences, University of Manchester, Manchester, UK</institution>
        </aff>
        <aff id="aff8"><label>8</label><institution>National Centre for Atmospheric Science, Fairbairn House, 71-75 Clarendon
Road, Leeds, LS2 9PH, UK</institution>
        </aff>
        <aff id="aff9"><label>9</label><institution>National Centre for Atmospheric Science, University of Manchester,
Manchester, UK</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Claire L. Ryder (c.l.ryder@reading.ac.uk)</corresp></author-notes><pub-date><day>6</day><month>December</month><year>2018</year></pub-date>
      
      <volume>18</volume>
      <issue>23</issue>
      <fpage>17225</fpage><lpage>17257</lpage>
      <history>
        <date date-type="received"><day>19</day><month>July</month><year>2018</year></date>
           <date date-type="rev-request"><day>6</day><month>August</month><year>2018</year></date>
           <date date-type="rev-recd"><day>9</day><month>November</month><year>2018</year></date>
           <date date-type="accepted"><day>13</day><month>November</month><year>2018</year></date>
      </history>
      <permissions>
        
        
      <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>
    <p id="d1e314">Mineral dust is an important component of the climate system, affecting the
radiation balance, cloud properties, biogeochemical cycles, regional
circulation and precipitation, as well as having negative effects on
aviation, solar energy generation and human health. Dust size and composition
has an impact on all these processes. However, changes in dust size
distribution and composition during transport, particularly for coarse
particles, are poorly understood and poorly represented in climate models.
Here we present new in situ airborne observations of dust in the Saharan Air
Layer (SAL) and the marine boundary layer (MBL) at the beginning of its
transatlantic transport pathway, from the AERosol
Properties – Dust (AER-D) fieldwork in August 2015,
within the peak season of North African dust export. This study focuses on
coarse-mode dust properties, including size distribution, mass loading,
shape, composition, refractive indices and optical properties. Size
distributions from 0.1 to 100 <inline-formula><mml:math id="M1" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter (<inline-formula><mml:math id="M2" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula>) are presented, fully
incorporating the coarse and giant modes of dust. Within the MBL, mean
effective diameter (<inline-formula><mml:math id="M3" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) and volume median diameter (VMD) were 4.6 and 6.0 <inline-formula><mml:math id="M4" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m respectively, giant particles with a mode at
20–30 <inline-formula><mml:math id="M5" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m were observed, and composition was dominated by quartz and
alumino-silicates at <inline-formula><mml:math id="M6" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 1 <inline-formula><mml:math id="M7" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Within the SAL, particles
larger than 20 <inline-formula><mml:math id="M8" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter were always present up to 5 km altitude, in
concentrations over 10<inline-formula><mml:math id="M9" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> cm<inline-formula><mml:math id="M10" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, constituting up to 40 % of
total dust mass. Mean <inline-formula><mml:math id="M11" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and VMD were 4.0 and 5.5 <inline-formula><mml:math id="M12" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
respectively. Larger particles were detected in the SAL than can be explained
by sedimentation theory alone. Coarse-mode composition was dominated by
quartz and alumino-silicates; the accumulation mode showed a strong
contribution from sulfate-rich and sea salt particles. In the SAL, measured
single scattering albedos (SSAs) at 550 nm representing <inline-formula><mml:math id="M13" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 2.5 <inline-formula><mml:math id="M14" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m were
0.93 to 0.98 (mean 0.97). Optical properties calculated for the full
size distribution (0.1 &lt; <inline-formula><mml:math id="M15" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 100 <inline-formula><mml:math id="M16" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) resulted in lower
SSAs of 0.91–0.98 (mean 0.95) and mass extinction coefficients of 0.27–0.35 m<inline-formula><mml:math id="M17" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> g<inline-formula><mml:math id="M18" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (mean 0.32 m<inline-formula><mml:math id="M19" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> g<inline-formula><mml:math id="M20" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>). Variability in SSA was mainly
controlled by variability in dust composition (principally iron) rather than
by variations in the size distribution, in contrast with previous observations
over the<?pagebreak page17226?> Sahara where size is the dominant influence. It is important that
models are able to capture the variability and evolution of both dust
composition and size distribution with transport in order to accurately
represent the impacts of dust on climate. These results provide a new SAL
dust dataset, fully representing coarse and giant particles, to aid model
validation and development.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p id="d1e499">Mineral dust plays an important role in the Earth's climate system. It is
the most dominant aerosol species in the atmosphere, constituting 70 % of
the global aerosol mass burden and 25 % of the aerosol optical depth (AOD)
(Kinne et al., 2006). Once uplifted from arid regions, dust is
transported thousands of kilometres across the Atlantic Ocean from the
Sahara (Carlson, 2016) and across the Pacific Ocean from
eastern Asian deserts (Li et al., 2010). The abundance and long-distance
transport of mineral dust allow it to affect the climate system via
different processes. Dust interacts with both solar and infrared radiation,
exerting a direct radiative effect at the top of atmosphere and surface,
which can alter atmospheric heating rates and stability, surface fluxes and
temperatures and thus influence regional circulation and precipitation
(Lavaysse et al., 2011; Strong et al., 2018). Dust particles may
influence cloud development on a microphysical level by acting as both cloud
condensation nuclei and ice nuclei (Kumar et al., 2011; Hoose and Mohler,
2012), affecting cloud optical properties and lifetimes. Finally, dust has
an impact on biogeochemical cycles since it provides iron to the ocean
(Jickells et al., 2005) and phosphorous to the Amazon rainforest (Yu
et al., 2015), which can lead to subsequent changes in atmospheric carbon
dioxide absorption by the oceans and vegetation and associated climate
feedbacks. Dust impacts anthropogenic activities by depleting solar
radiation available for solar energy generation, both in the atmosphere
(Charabi and Gastli, 2012) and by deposition to solar panels
(Piedra and Moosmuller, 2017). It also negatively impacts aviation
in dust-laden regions due to a reduction in visibility (Middleton,
2017), and finally high dust loadings can negatively impact respiratory
health (Prospero et al., 2014). Many of these processes are dependent not
only on the total mass of dust but also its size (Mahowald et al., 2014).</p>
      <p id="d1e502">Recent studies have revealed how poorly climate models are able to simulate the uplift and transport of dust. Evan et al. (2014) find that CMIP5
climate models underestimate the dust mass path (the mass loading of dust per
square metre) by a factor of 3, 66 % of which is due to a bias in size
distribution skewed towards smaller particles and 34 % of which is due to
an underestimate in emission fluxes. As a result, these models
systematically failed to reproduce basic aspects of dust emission and
transport, casting doubt on their ability to simulate regional African
climate and the response of African dust to future climate change. Kok et al. (2017) used an observationally constrained emitted dust size
distribution in combination with global model simulations to determine dust
radiative forcing. They estimated a more positive radiative forcing (<inline-formula><mml:math id="M21" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.48</mml:mn></mml:mrow></mml:math></inline-formula>
to <inline-formula><mml:math id="M22" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>0.20 Wm<inline-formula><mml:math id="M23" 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>) compared to previous estimates from the AeroCom models
(<inline-formula><mml:math id="M24" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.6</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M25" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.3</mml:mn></mml:mrow></mml:math></inline-formula> Wm<inline-formula><mml:math id="M26" 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>) which over-represented smaller, more cooling
particles and under-represented the coarser, more warming particles. Kim
et al. (2014) compared AeroCom models to satellite data and found disagreement in dust optical depth of up to a factor of 4, also finding
that the mass extinction coefficient (MEC, which is sensitive to particle size
distribution) varied by 27 % between models. These studies emphasize the
sensitivity of model predictions of key parts of the climate system to the representation of particle size and the challenges of capturing
observations in current climate models.</p>
      <p id="d1e567">Coarse- and giant-mode dust (defined here as <inline-formula><mml:math id="M27" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 2.5 and
<inline-formula><mml:math id="M28" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 20 <inline-formula><mml:math id="M29" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m respectively) is of particular importance to its
interaction with radiation. In the shortwave (SW) spectrum, larger particles
(assuming fixed composition, shape and roughness) increase the amount of
atmospheric absorption, thus decreasing the single scattering albedo (SSA or
<inline-formula><mml:math id="M30" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ω</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) (Tegen and Lacis, 1996). For example, calculations
have shown that including coarse- and giant-mode particles measured over the
Sahara results in the SSA dropping from 0.92 to 0.80 at 500 nm. This
resulted in the associated atmospheric heating rates increasing by up to a
factor of 3 (Ryder et al., 2013b). In the longwave (LW) spectrum,
coarse particles are equally important. Otto et al. (2011) show that
including particles larger than 5 <inline-formula><mml:math id="M31" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter more than doubles the
dust LW AOD; and the magnitude of the LW radiative effect can act to change
the sign of the net radiative effect of dust (Woodage and Woodward,
2014). Song et al. (2018) show that dust radiative closure assessed by
satellite observations in both the shortwave and longwave spectra can only
be achieved with a substantial coarse-mode dust size distribution.</p>
      <p id="d1e609">Part of the challenge in modelling the dust cycle is that it is not
currently clear even from observations what all the mechanisms for the
transport of coarse particles are. In theory, dry deposition depends on
particle size but is also influenced by particle shape, density and
roughness (Li and Osada, 2007). However, observations have
consistently shown that coarse dust particles are transported further than
predicted by dry-deposition theory (Maring et al., 2003; Ryder et al.,
2013a; Weinzierl et al., 2017; Gasteiger et al., 2017; Denjean et al., 2016;
Stevenson et al., 2015). Various suggestions as to the observed retention of
the coarse mode during transport have been proposed, including solar
absorption by dust generating convection and therefore additional vertical
mixing in dust layers (e.g. Gasteiger et al., 2017), turbulence within
dust layers (Denjean et al., 2016), and electrostatic charging of dust
(Harrison et al., 2018). Measuring and quantifying these
processes remains challenging. In order to do so, high-quality<?pagebreak page17227?> observations
of dust properties at multiple stages throughout transport events are
required.</p>

<?xmltex \floatpos{p}?><table-wrap id="Ch1.T1" specific-use="star"><caption><p id="d1e616">Airborne campaigns measuring size distributions of Saharan mineral
dust since 2006, showing maximum particle size measured and size
restrictions by inlets where instruments were located inside the aircraft
cabin. OPC size ranges are nominal diameters. See text for abbreviations. APS: aerodynamic particle
sampler; CAS-DPOL: cloud and aerosol spectrometer with depolarization
detection; FSSP: forward scattering spectrometer probe; SID: small ice detector.</p></caption><oasis:table frame="topbot"><?xmltex \begin{scaleboxenv}{.90}[.90]?><oasis:tgroup cols="9">
     <oasis:colspec colnum="1" colname="col1" align="justify" colwidth="75pt"/>
     <oasis:colspec colnum="2" colname="col2" align="justify" colwidth="49pt"/>
     <oasis:colspec colnum="3" colname="col3" align="justify" colwidth="35pt"/>
     <oasis:colspec colnum="4" colname="col4" align="justify" colwidth="45pt"/>
     <oasis:colspec colnum="5" colname="col5" align="justify" colwidth="42.679134pt"/>
     <oasis:colspec colnum="6" colname="col6" align="justify" colwidth="25pt"/>
     <oasis:colspec colnum="7" colname="col7" align="justify" colwidth="40pt"/>
     <oasis:colspec colnum="8" colname="col8" align="justify" colwidth="100pt"/>
     <oasis:colspec colnum="9" colname="col9" align="justify" colwidth="50pt"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Campaign</oasis:entry>
         <oasis:entry colname="col2">Abbreviation</oasis:entry>
         <oasis:entry colname="col3">Fieldwork date</oasis:entry>
         <oasis:entry colname="col4">Location</oasis:entry>
         <oasis:entry colname="col5">Measurement upper size<?xmltex \hack{\hfill\break}?>limit, <inline-formula><mml:math id="M32" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m</oasis:entry>
         <oasis:entry colname="col6">Instru-<?xmltex \hack{\hfill\break}?>ment type</oasis:entry>
         <oasis:entry colname="col7">In-cabin or wing-<?xmltex \hack{\hfill\break}?>mounted</oasis:entry>
         <oasis:entry colname="col8">Details</oasis:entry>
         <oasis:entry colname="col9">Publication</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Dust And Biomass<?xmltex \hack{\hfill\break}?>burning Experiment</oasis:entry>
         <oasis:entry colname="col2">DABEX</oasis:entry>
         <oasis:entry colname="col3">2006</oasis:entry>
         <oasis:entry colname="col4">Niger</oasis:entry>
         <oasis:entry rowsep="1" colname="col5">10</oasis:entry>
         <oasis:entry rowsep="1" colname="col6">OPC</oasis:entry>
         <oasis:entry rowsep="1" colname="col7">In-cabin</oasis:entry>
         <oasis:entry rowsep="1" colname="col8">PCASP-X, behind a<?xmltex \hack{\hfill\break}?>counter-flow virtual im-<?xmltex \hack{\hfill\break}?>pactor with significant<?xmltex \hack{\hfill\break}?>pipework; loss of majority<?xmltex \hack{\hfill\break}?>of coarse particles</oasis:entry>
         <oasis:entry rowsep="1" colname="col9">Osborne et<?xmltex \hack{\hfill\break}?>al. (2008)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5">10</oasis:entry>
         <oasis:entry colname="col6">Filter samples</oasis:entry>
         <oasis:entry colname="col7">In-cabin</oasis:entry>
         <oasis:entry colname="col8">Inlet restricted measure-<?xmltex \hack{\hfill\break}?>ments to 35 % of coarse<?xmltex \hack{\hfill\break}?>mode (<inline-formula><mml:math id="M33" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 1.4 <inline-formula><mml:math id="M34" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m)</oasis:entry>
         <oasis:entry colname="col9">Chou et<?xmltex \hack{\hfill\break}?>al. (2008)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Dust Outflow and<?xmltex \hack{\hfill\break}?>Deposition to the<?xmltex \hack{\hfill\break}?>Ocean 2</oasis:entry>
         <oasis:entry colname="col2">DODO2</oasis:entry>
         <oasis:entry colname="col3">Aug 2006</oasis:entry>
         <oasis:entry colname="col4">Tropical eastern Atlantic</oasis:entry>
         <oasis:entry colname="col5">40</oasis:entry>
         <oasis:entry colname="col6">OPC</oasis:entry>
         <oasis:entry colname="col7">Wing-mounted</oasis:entry>
         <oasis:entry colname="col8">CDP measurements on a<?xmltex \hack{\hfill\break}?>few flights only; otherwise<?xmltex \hack{\hfill\break}?>size distributions up to 3 <inline-formula><mml:math id="M35" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m</oasis:entry>
         <oasis:entry colname="col9">McConnell et<?xmltex \hack{\hfill\break}?>al. (2008)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">African Monsoon<?xmltex \hack{\hfill\break}?>Multidisciplinary Analysis</oasis:entry>
         <oasis:entry colname="col2">AMMA</oasis:entry>
         <oasis:entry colname="col3">Jun–Jul 2006</oasis:entry>
         <oasis:entry colname="col4">Niger and<?xmltex \hack{\hfill\break}?>Benin</oasis:entry>
         <oasis:entry colname="col5">20</oasis:entry>
         <oasis:entry colname="col6">OPC</oasis:entry>
         <oasis:entry colname="col7">In-cabin</oasis:entry>
         <oasis:entry colname="col8">Grimm OPC behind isokinetic inlet with 50 % passing efficiency at 9 <inline-formula><mml:math id="M36" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m</oasis:entry>
         <oasis:entry colname="col9">Formenti et<?xmltex \hack{\hfill\break}?>al. (2011)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">NASA AMMA</oasis:entry>
         <oasis:entry colname="col2">NAMMA</oasis:entry>
         <oasis:entry colname="col3">Aug–Sep 2006</oasis:entry>
         <oasis:entry colname="col4">Tropical eastern Atlantic</oasis:entry>
         <oasis:entry colname="col5">5</oasis:entry>
         <oasis:entry colname="col6">APS</oasis:entry>
         <oasis:entry colname="col7">In-cabin</oasis:entry>
         <oasis:entry colname="col8">APS behind an inlet with<?xmltex \hack{\hfill\break}?>50 % sampling efficiency at<?xmltex \hack{\hfill\break}?>5 <inline-formula><mml:math id="M37" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m</oasis:entry>
         <oasis:entry colname="col9">Chen et<?xmltex \hack{\hfill\break}?>al. (2011)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Saharan Mineral<?xmltex \hack{\hfill\break}?>Dust Experiment 1</oasis:entry>
         <oasis:entry colname="col2">SAMUM1</oasis:entry>
         <oasis:entry colname="col3">May–Jun 2006</oasis:entry>
         <oasis:entry colname="col4">Morocco</oasis:entry>
         <oasis:entry colname="col5">30/<?xmltex \hack{\hfill\break}?>100</oasis:entry>
         <oasis:entry colname="col6">OPCs</oasis:entry>
         <oasis:entry colname="col7">Wing-mounted</oasis:entry>
         <oasis:entry colname="col8">FSSP-300/FSSP-100</oasis:entry>
         <oasis:entry colname="col9">Weinzierl et<?xmltex \hack{\hfill\break}?>al. (2009)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Geostationary Earth<?xmltex \hack{\hfill\break}?>Radiation Budget<?xmltex \hack{\hfill\break}?>Intercomparison of<?xmltex \hack{\hfill\break}?>Longwave and<?xmltex \hack{\hfill\break}?>Shortwave radiation</oasis:entry>
         <oasis:entry colname="col2">GERBILS</oasis:entry>
         <oasis:entry colname="col3">Jun 2007</oasis:entry>
         <oasis:entry colname="col4">Mali, Southern Mauritania</oasis:entry>
         <oasis:entry colname="col5">60</oasis:entry>
         <oasis:entry colname="col6">OPC</oasis:entry>
         <oasis:entry colname="col7">Wing-mounted</oasis:entry>
         <oasis:entry colname="col8">SID-2; PSDs represent<?xmltex \hack{\hfill\break}?>aged, transported dust<?xmltex \hack{\hfill\break}?>events with light dust<?xmltex \hack{\hfill\break}?>loadings</oasis:entry>
         <oasis:entry colname="col9">Johnson and<?xmltex \hack{\hfill\break}?>Osborne (2011)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Saharan Mineral<?xmltex \hack{\hfill\break}?>Dust Experiment 2</oasis:entry>
         <oasis:entry colname="col2">SAMUM2</oasis:entry>
         <oasis:entry colname="col3">Jan–Feb 2008</oasis:entry>
         <oasis:entry colname="col4">Tropical eastern Atlantic</oasis:entry>
         <oasis:entry colname="col5">30</oasis:entry>
         <oasis:entry colname="col6">OPC</oasis:entry>
         <oasis:entry colname="col7">Wing-mounted</oasis:entry>
         <oasis:entry colname="col8">FSSP-300</oasis:entry>
         <oasis:entry colname="col9">Weinzierl et<?xmltex \hack{\hfill\break}?>al. (2011)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Fennec – The Sa- <?xmltex \hack{\hfill\break}?>haran Climate Sys-<?xmltex \hack{\hfill\break}?>tem</oasis:entry>
         <oasis:entry colname="col2">Fennec</oasis:entry>
         <oasis:entry colname="col3">Jun 2011</oasis:entry>
         <oasis:entry colname="col4">Mali, Mau- <?xmltex \hack{\hfill\break}?>ritania</oasis:entry>
         <oasis:entry colname="col5">50/<?xmltex \hack{\hfill\break}?>60/<?xmltex \hack{\hfill\break}?>930</oasis:entry>
         <oasis:entry colname="col6">OPCs and OAPs</oasis:entry>
         <oasis:entry colname="col7">Wing-mounted</oasis:entry>
         <oasis:entry colname="col8">CDP/SID2/CIP15</oasis:entry>
         <oasis:entry colname="col9">Ryder et<?xmltex \hack{\hfill\break}?>al. (2013b)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Aerosol Direct Ra-<?xmltex \hack{\hfill\break}?>diative Impact on the<?xmltex \hack{\hfill\break}?>regional climate in <?xmltex \hack{\hfill\break}?>the MEDiterranean<?xmltex \hack{\hfill\break}?>region</oasis:entry>
         <oasis:entry colname="col2">ADRIMED</oasis:entry>
         <oasis:entry colname="col3">Jun–Jul 2013</oasis:entry>
         <oasis:entry colname="col4">Mediterranean Sea</oasis:entry>
         <oasis:entry colname="col5">20</oasis:entry>
         <oasis:entry colname="col6">OPC</oasis:entry>
         <oasis:entry colname="col7">Wing-mounted</oasis:entry>
         <oasis:entry colname="col8">FSSP-300</oasis:entry>
         <oasis:entry colname="col9">Denjean et<?xmltex \hack{\hfill\break}?>al. (2016)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Saharan Aerosol<?xmltex \hack{\hfill\break}?>Long-range Trans-<?xmltex \hack{\hfill\break}?>port and Aerosol-<?xmltex \hack{\hfill\break}?>Cloud-Interaction Experiment</oasis:entry>
         <oasis:entry colname="col2">SALTRACE</oasis:entry>
         <oasis:entry colname="col3">Jun–Jul 2013</oasis:entry>
         <oasis:entry colname="col4">Tropical western Atlantic</oasis:entry>
         <oasis:entry colname="col5">50/100</oasis:entry>
         <oasis:entry colname="col6">OPCs</oasis:entry>
         <oasis:entry colname="col7">Wing-mounted</oasis:entry>
         <oasis:entry colname="col8">CAS-DPOL/FSSP-100. Some measurements ad-<?xmltex \hack{\hfill\break}?>ditionally taken over the<?xmltex \hack{\hfill\break}?>eastern tropical Atlantic</oasis:entry>
         <oasis:entry colname="col9">Weinzierl et<?xmltex \hack{\hfill\break}?>al. (2017)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">AERosol Properties<?xmltex \hack{\hfill\break}?>– Dust</oasis:entry>
         <oasis:entry colname="col2">AER-D</oasis:entry>
         <oasis:entry colname="col3">Aug 2015</oasis:entry>
         <oasis:entry colname="col4">Tropical eastern Atlantic</oasis:entry>
         <oasis:entry colname="col5">100</oasis:entry>
         <oasis:entry colname="col6">OPCs and OAPs</oasis:entry>
         <oasis:entry colname="col7">Wing-mounted</oasis:entry>
         <oasis:entry colname="col8">CDP, CIP15 and 2-DS</oasis:entry>
         <oasis:entry colname="col9">This article</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup><?xmltex \end{scaleboxenv}?></oasis:table></table-wrap>

      <p id="d1e1201">Over the last 15 years, aircraft observations have made significant advances
both in observing dust in increasingly remote regions of the Sahara near
dust sources and in utilizing instrumentation to characterize the full dust
size distribution. The major fieldwork campaigns since 2005 are shown in
Table 1, including the measurement technique and
maximum size measured. Size distributions can be measured inside aircraft
cabins behind inlets, although this introduces restrictions enforced by
inlet-dependent size cuts which prevent the measurement of the coarser
particles to varying degrees. In recent years, wing-mounted sizing probes
have been more routinely operated, removing any inlet sizing restrictions.
Wing probes have employed both light scattering and light-shadowing
techniques. Optical particle counters (OPCs) measure light scattering, and
post-processing requires converting scattering cross section to particle
size. This relationship, although dominated by particle size, is also
impacted by aerosol composition (via the refractive index), and the
scattering cross section to particle size relationship is non-monotonic.
Non-spherical particles may also impact the retrieved size distribution.
These limitations, impacts and uncertainties are discussed in detail by
Ryder et al. (2015). Optical array probes (OAPs) can be wing-mounted and
utilize light-shadowing techniques for particle sizing and are not subject
to the above uncertainties and therefore present a valuable method for the sizing of coarse dust particles, as demonstrated by Ryder et al. (2013b), although sizing can still be subject to uncertainties, such as from
particle shape. All wing probes can also potentially suffer from
modification of the flow around the probe housing and particle bouncing from
the probe tips (Korolev et al., 2013; Weigel et al., 2016; McFarquhar et
al., 2017).</p>
      <p id="d1e1204">The progressive airborne measurement of larger dust particle sizes has
demonstrated the prevalence of coarse and giant particles both over desert
regions and far from sources. For example, Weinzierl et al. (2009)
detected particles larger than 40 <inline-formula><mml:math id="M38" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m in 20 % of cases over Morocco
during the Saharan Mineral Dust Experiment (SAMUM1), even up to 5 km altitude. During Fennec, dust particles sized
over 100 <inline-formula><mml:math id="M39" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m were measured at altitudes up to 5 km over Mali and
Mauritania (Ryder et al., 2013b). During SAMUM2 over the Atlantic Ocean,
although dust particles sized over 10 <inline-formula><mml:math id="M40" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m were present in 88 % of
cases, no particles sized over 30 <inline-formula><mml:math id="M41" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m were detected (Weinzierl et
al., 2011). However, these observations were performed within the low-altitude wintertime Saharan dust plume (under 1.5 km), whereas the
summertime elevated dust plume within the Saharan Air Layer (SAL) is subject
to different meteorological and dust uplift and transport mechanisms
(Prospero and Carlson, 1972; Karyampudi et al., 1999; McConnell et al.,
2008).</p>
      <p id="d1e1235">Here we present new airborne measurements of aerosol in the tropical eastern
Atlantic region, obtained during August 2015 as part of the AERosol
Properties – Dust (AER-D) fieldwork campaign, which ran alongside the Ice
in Clouds Experiment – Dust (ICE-D) project. We utilize size distribution
instrumentation aboard the UK FAAM BAe 146 research aircraft consistent with
the Fennec campaigns of 2011 and 2012 (Ryder et al., 2015) and present
dust properties measured during summer, the peak North African dust
transport season (Doherty et al., 2008), with a particular focus on
the properties of the coarse mode. New real-time measurements of
accumulation mode hematite content measured during several of the same
flights, and their optical properties, are presented separately by Liu et al. (2018). Ice nucleating properties of the dust sampled are given by
Price et al. (2018), and the vertical structure is analysed by
Marenco et al. (2018).</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T2" specific-use="star"><caption><p id="d1e1241">Dates of AER-D flights and times of intensive in situ sampling
SLRs and accumulation mode AOD at the region of in situ sampling.</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="left"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="left"/>
     <oasis:thead>
       <oasis:row>
         <oasis:entry colname="col1">Flight</oasis:entry>
         <oasis:entry colname="col2">Date</oasis:entry>
         <oasis:entry colname="col3">Times of in situ</oasis:entry>
         <oasis:entry colname="col4">Accumulation mode</oasis:entry>
         <oasis:entry colname="col5">General flight</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">number</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">sampling (UTC)</oasis:entry>
         <oasis:entry colname="col4">550 nm AOD</oasis:entry>
         <oasis:entry colname="col5">aims and conditions</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">b920</oasis:entry>
         <oasis:entry colname="col2">7 Aug 2015</oasis:entry>
         <oasis:entry colname="col3">15:00–17:00</oasis:entry>
         <oasis:entry colname="col4">0.4</oasis:entry>
         <oasis:entry colname="col5">In situ and remote sensing,</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5">CATS underflight</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">b923</oasis:entry>
         <oasis:entry colname="col2">12 Aug 2015</oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">1.8<inline-formula><mml:math id="M43" display="inline"><mml:msup><mml:mi/><mml:mo>*</mml:mo></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col5">High-level remote sensing of dust, mapping of intense dust</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5">event, Cape Verde to Fuerteventura, Canary Islands</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">b924</oasis:entry>
         <oasis:entry colname="col2">12 Aug 2015</oasis:entry>
         <oasis:entry colname="col3">15:30–16:30</oasis:entry>
         <oasis:entry colname="col4">2.5</oasis:entry>
         <oasis:entry colname="col5">In situ and remote sensing of intense dust event,</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5">Fuerteventura, Canary Islands to Cape Verde</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">b928</oasis:entry>
         <oasis:entry colname="col2">16 Aug 2015</oasis:entry>
         <oasis:entry colname="col3">15:00–18:00</oasis:entry>
         <oasis:entry colname="col4">0.8</oasis:entry>
         <oasis:entry colname="col5">SAVEX-D flight 1; in situ and remote sensing</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5">close to Praia ground site</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">b932</oasis:entry>
         <oasis:entry colname="col2">20 Aug 2015</oasis:entry>
         <oasis:entry colname="col3">11:00–12:00</oasis:entry>
         <oasis:entry colname="col4">0.7</oasis:entry>
         <oasis:entry colname="col5">In situ and remote sensing</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">b934</oasis:entry>
         <oasis:entry colname="col2">25 Aug 2015</oasis:entry>
         <oasis:entry colname="col3">15:00–17:45</oasis:entry>
         <oasis:entry colname="col4">0.6</oasis:entry>
         <oasis:entry colname="col5">SAVEX-D flight 2; in situ and remote</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5">sensing close to Sal ground site</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><table-wrap-foot><p id="d1e1244"><inline-formula><mml:math id="M42" display="inline"><mml:msup><mml:mi/><mml:mo>*</mml:mo></mml:msup></mml:math></inline-formula> No in situ sampling, AOD is provided at the Canary Islands.</p></table-wrap-foot></table-wrap>

</sec>
<sec id="Ch1.S2">
  <title>Method</title>
<sec id="Ch1.S2.SS1">
  <title>Flight patterns</title>
      <p id="d1e1509">During August 2015, the UK BAe 146-301 Research Aircraft operated by the
Facility for Airborne Atmospheric Measurements was stationed at Praia on the
Cape Verde islands, for the ICE-D and AER-D field campaigns. The AER-D
project comprised six flights, focusing specifically on dust properties
within and beneath the SAL. Each flight was performed 4 to 5 days apart, due
to the transported dust in the SAL displaying intermittent character,
typical for summertime dust export (Jones et al., 2003; Schepanski et
al., 2017). Details of the flights are shown in
Table 2, and flight tracks are shown in
Fig. 1.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><caption><p id="d1e1514">Map showing the location of the AER-D flights, out of Praia
on Cape Verde. Thin lines show full flight tracks; bold sections indicate
in situ sampling SLRs analysed here. Note that within each flight there were
several SLRs at different altitudes, which overlie each other here. Circles
indicate dust source locations. Numbers indicate primary, secondary and
tertiary dust uplift (see Table 4) events. Note
that flights b923/b924 sampled the same dust event.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f01.pdf"/>

        </fig>

      <p id="d1e1523">The events sampled revealed accumulation mode AODs at 550 nm (see Sect. 2.3.1) from 0.4 to 0.8, which is within the range
expected from August climatology over the eastern tropical Atlantic
indicated by satellite imagery (not shown). The aircraft observations
revealed a mostly typical vertical dust structure (see Sect. 3.1). The exceptions were b923 and b924, a pair of
flights which observed an intense dust outbreak with AODs of up to 2.5 at
around 24<inline-formula><mml:math id="M44" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N off the coast of West Africa, with in situ and remote-sensing
observations showing a different and complex vertical structure compared to
the conventional SAL model of an elevated dust layer (discussed in
Marenco et al., 2018).</p>
      <?pagebreak page17229?><p id="d1e1535">Two flights (b928, b934) formed part of the Sunphotometer Airborne
Validation Experiment in AER-D (SAVEX-D) project, focused on providing
airborne measurements for comparison with two types of ground-based
sun photometer. Requirements for non-cloudy skies and moderate to high dust
loadings and proximity to the ground-based sun photometers required that the
first SAVEX-D flight (b928) took place close to Praia, while the second
(b934) took place close to the island of Sal. Three flights (b923, b924 and
b932) were aimed mainly at mapping the vertical and horizontal aerosol
structure. These flights headed to the northeast in order to encounter heavy
dust loads closer to the African coast on 12 August. Flight b920 was
conducted near the Cape Verde archipelago and co-located with the path of
the International Space Station (ISS), in order to fully characterize the
SAL and validate the Cloud-Aerosol Transport System (CATS) remote-sensing
lidar instrument onboard the ISS.</p>
      <p id="d1e1539">Each flight consists of a combination of sloped profiles (abbreviated to
“P”, e.g. “P1”) and straight-and-level runs (known as “SLRs” and abbreviated
to “R”, e.g. “R2”) at various altitudes, generally selected to be within the
aerosol layer of interest or at altitudes appropriate for radiometric
measurements. Here we present results from 31 profiles and 19 in situ
aerosol sampling SLRs, as shown in Fig. 1. Five
SLRs were performed in the marine boundary layer (MBL) at 30 to 35 m above
sea level (one per flight), and 14 SLRs sampled the SAL at altitudes between
1.8 and 4.1 km. Exceptions were an intermediate layer sampled during flight
b920<?pagebreak page17230?> containing dust at 1.2 km and heavy dust sampled during flight b924 at
920 m. Full information about profile and SLR times and altitude are
available from the Centre for Environmental Data Analysis (see
the “data availability” section).</p>
</sec>
<sec id="Ch1.S2.SS2">
  <title>Determination of dust sources and dust age</title>
      <p id="d1e1548">Broad geographic dust source locations, where dust was uplifted before being
sampled by the aircraft during AER-D, have been identified using Spinning
Enhanced Visible and Infrared Imager (SEVIRI) “dust RGB” (red–green–blue)
thermal infrared satellite imagery product (Lensky and Rosenfeld,
2008), where dust events are identifiable by their bright pink colour (e.g.
Brindley et al., 2012). Dust events sampled by the aircraft are tracked
backwards in time visually until uplift times and locations are identified,
identical to Ryder et al. (2013b). The high temporal resolution (15 min)
of the imagery enables easier tracking compared to other spaceborne sensors
which may have only two overpasses per day. However, this method is
subjective, and therefore we allow generous errors in terms of geographic
dust uplift location, and dust uplift time. Additionally, no height
resolution information is available from the imagery, so source areas are
categorized for each flight and not for each sampling altitude within
flights.</p>
      <p id="d1e1551">The examination the dust events sampled during AER-D reveals that the dust in
every event was initially uplifted by a mesoscale convective system (MCS)
and a resultant cold pool (haboob) which spread out radially. This is in
keeping with recent findings that cold pools are the dominant mechanism for
summertime Saharan dust uplift (Marsham et al., 2013; Allen et al.,
2013). The dust events then took 1 to 5 days to reach the Atlantic Ocean
where they were sampled by the aircraft. In three cases, additional uplift
events could be observed merging with the initial dust event, and in these
cases error bounds on dust age were set to include all possible uplift
events and were therefore very broad. In most cases, convection and clouds
could be observed developing over the SAL during the afternoon in the top of
the dust layers during their transport. Therefore, it is possible that the
dust observed has been processed by clouds (e.g. Ryder et al., 2015
Sect. 4.1.4; Diaz-Hernandez and Sanchez-Navas, 2016), though no
clouds were present when sampling took place.</p>
      <p id="d1e1554">The SEVIRI imagery is not able to give altitude-resolved information and
can be subjective, particularly when dust loadings are light, at low
altitude or in a moist environment, making dust appear less pink and more
difficult to identify (Brindley et al., 2012). This is more evident in
the dust tracked for flights b932 and b934 where dust loadings were lower.
This introduces a small level of uncertainty into both the source locations
and dust ages, which we account for by giving generous error bars to the
dust uplift times and source locations. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories
(Draxler and Hess, 1998; Stein et al., 2015) were also run for the AER-D
dust events. In only one of the five dust events was the dust source
location similar to that observed in the SEVIRI imagery. In every case the
back trajectories indicated a transport path and transport time different to
that shown by the SEVIRI imagery. Although the SEVIRI methodology has its
limitations, the back-trajectory method results were clearly not compatible
with the information from SEVIRI. Therefore, back trajectories are not used
to determine source location or age here. Additionally, another limitation
of back trajectories is that they only indicate when an air mass nears the
surface but do not reflect potential uplift conditions (e.g. surface wind
strength or soil conditions). It has been shown that models and reanalyses
are currently unable to adequately represent convective events and winds
over the Sahara and Sahel, particularly due to the challenges of
representing cold pools. For example, Garcia-Carreras et al. (2013)
examine the role of convective cold pools and suggest that “the
misrepresentation of moist convective processes can affect continental-scale
biases, altering the West African monsoon circulation.” Many other
publications have examined the misrepresentation of Saharan convective
events (Marsham et al., 2011; Heinold et al., 2009; Sodemann et al.,
2015; Trzeciak et al., 2017; Allen et al., 2015; Roberts et al., 2017;
Engelstaedter et al., 2015). Since convective events are the drivers of dust
uplift in all the AER-D cases, we do not consider HYSPLIT back trajectories
(with relatively low model resolution of half a degree) to be informative
here due to the challenges the models face in representing Saharan
circulation. Finally, we note that back trajectories are recommended to be
used with caution for dust events over the summertime Sahara
(Trzeciak et al., 2017).</p>
</sec>
<sec id="Ch1.S2.SS3">
  <title>Instrumentation</title>
      <p id="d1e1563">Much of the instrumentation operated during ICE-D was identical to that
operated during the Fennec campaign, described in Ryder et al. (2013b, 2015). Relevant information is provided below, noting
where instruments and processing differed. Throughout this article all
particle sizes are referred to in terms of diameter (<inline-formula><mml:math id="M45" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula>), and optical
properties are presented at 550 nm unless stated otherwise.</p>
<sec id="Ch1.S2.SS3.SSS1">
  <title>Inlets, scattering and absorption measurements</title>
      <p id="d1e1578">Scattering measurements were made by a TSI 3563 integrating nephelometer (at
wavelengths of 450, 550 and 700 nm). Absorption measurements were made by a
Radiance Research particle soot absorption photometer (PSAP) at 567 nm. Both
instruments are situated inside the aircraft cabin, behind a modified
Rosemount 102E inlet. PSAP filters were changed before every flight and spot
size was measured. Standard corrections are performed on both instruments.
For the PSAP these are taken from Turnbull (2010), which
incorporates corrections necessary to the FAAM PSAP<?pagebreak page17231?> measurements based on
the original work by Bond et al. (1999), and further clarifications to
this publication described by Ogren (2010). For the nephelometer, corrections are performed according to Anderson and Ogren (1998)
assuming supermicron particles. This results in 11 % and 15 %
uncertainty in extinction and SSA respectively
(Ryder et al., 2013b). Corrections for internal nephelometer temperature
and pressure are included.</p>
      <p id="d1e1581">Accumulation mode AODs are calculated from aircraft profiles by integrating
the scattering and absorption measurements between the minimum aircraft
altitude (typically around 30 m a.s.l.) to the top of the profile
(typically around 6 km). Therefore, AODs represent both SAL and MBL aerosol.</p>
      <p id="d1e1584">Extensive experimental and theoretical efforts to characterize inlet and
pipe losses were performed during Fennec (Trembath, 2012; Ryder et al.,
2013b), and we apply those results here. It was found that the net impact of
both Rosemount inlets and pipework supplying the nephelometer and PSAP led
to number concentration enhancements by a factor of 1.5 for <inline-formula><mml:math id="M46" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 1.5 <inline-formula><mml:math id="M47" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, no net loss or enhancement at 2.5 <inline-formula><mml:math id="M48" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, net losses between
2.5 to 5 <inline-formula><mml:math id="M49" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (50 % efficiency at <inline-formula><mml:math id="M50" display="inline"><mml:mrow><mml:mn mathvariant="normal">3.5</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M51" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m), and no
particles larger than 5 <inline-formula><mml:math id="M52" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m sampled. The exact enhancement and losses
vary between the nephelometer and PSAP (slightly different pipework) and
with altitude (see Supplement Fig. S1). Since it is clear that coarse-mode
particles do not reach the nephelometer and PSAP, henceforward the term
“accumulation mode” is used to describe the size distribution arriving at
these two instruments, roughly representing particles sized <inline-formula><mml:math id="M53" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 2.5 <inline-formula><mml:math id="M54" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. The enhancement and loss factors as a function of diameter are
applied to the size distribution described in Sect. 2.3.2 in order to replicate the accumulation mode
size distributions reaching the nephelometer and PSAP.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T3" specific-use="star"><caption><p id="d1e1659">Wing-mounted size distribution instrumentation operated during
AER-D; n/a – not applicable.</p></caption><oasis:table frame="topbot"><?xmltex \begin{scaleboxenv}{.82}[.82]?><oasis:tgroup cols="7">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="left"/>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Instrument</oasis:entry>
         <oasis:entry colname="col2">Abbreviation</oasis:entry>
         <oasis:entry colname="col3">Wavelength,</oasis:entry>
         <oasis:entry colname="col4">Scattering angle, degrees</oasis:entry>
         <oasis:entry colname="col5">Nominal size range</oasis:entry>
         <oasis:entry colname="col6">Corrected size range,</oasis:entry>
         <oasis:entry colname="col7">Measurement</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">nm</oasis:entry>
         <oasis:entry colname="col4">(primary, secondary)</oasis:entry>
         <oasis:entry colname="col5">measured, <inline-formula><mml:math id="M55" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M56" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter</oasis:entry>
         <oasis:entry colname="col7">method</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Passive cavity aerosol</oasis:entry>
         <oasis:entry colname="col2">PCASP</oasis:entry>
         <oasis:entry colname="col3">632.8</oasis:entry>
         <oasis:entry colname="col4">35–120, 60–145</oasis:entry>
         <oasis:entry colname="col5">0.1–3.0</oasis:entry>
         <oasis:entry colname="col6">0.12–3.02</oasis:entry>
         <oasis:entry colname="col7">Light scattering</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">spectrometer probe 100-X</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Cloud Droplet Probe</oasis:entry>
         <oasis:entry colname="col2">CDP</oasis:entry>
         <oasis:entry colname="col3">658</oasis:entry>
         <oasis:entry colname="col4">1.7–14</oasis:entry>
         <oasis:entry colname="col5">3–50</oasis:entry>
         <oasis:entry colname="col6">3.4–95.4</oasis:entry>
         <oasis:entry colname="col7">Light scattering</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Cloud Imaging Probe 15</oasis:entry>
         <oasis:entry colname="col2">CIP15</oasis:entry>
         <oasis:entry colname="col3">642</oasis:entry>
         <oasis:entry colname="col4">n/a</oasis:entry>
         <oasis:entry colname="col5">15–930</oasis:entry>
         <oasis:entry colname="col6">n/a</oasis:entry>
         <oasis:entry colname="col7">Light shadowing</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Two-dimensional stereo probe</oasis:entry>
         <oasis:entry colname="col2">2-DS</oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">n/a</oasis:entry>
         <oasis:entry colname="col5">10–1280</oasis:entry>
         <oasis:entry colname="col6">n/a</oasis:entry>
         <oasis:entry colname="col7">Light shadowing</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Cloud Imaging Probe 100</oasis:entry>
         <oasis:entry colname="col2">CIP100</oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">n/a</oasis:entry>
         <oasis:entry colname="col5">100–6200</oasis:entry>
         <oasis:entry colname="col6">n/a</oasis:entry>
         <oasis:entry colname="col7">Light shadowing</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup><?xmltex \end{scaleboxenv}?></oasis:table></table-wrap>

</sec>
<sec id="Ch1.S2.SS3.SSS2">
  <title>Size distribution measurements</title>
      <p id="d1e1895">We present size distribution measurements from a combination of different
wing-mounted instruments as shown in Table 3. We
utilize optical particle counter techniques for the accumulation and coarse
modes (passive cavity aerosol spectrometer probe (PCASP) and Cloud Droplet
Probe (CDP)) and light-shadowing measurement techniques for the giant mode
(two-dimensional stereo probe (2-DS), Cloud Imaging Probe 15 (CIP15), Cloud
Imaging Probe 100 (CIP100)). Size distributions are also provided for some
SLRs from filter sample analysis (Sect. 2.4).
This range of instrumentation allows us to take advantage of measuring a
wide particle size range (0.1 to 6200 <inline-formula><mml:math id="M57" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m), though the processing and
uncertainties associated with each must be considered carefully, as follows.
Uncertainties due to flow distortion effects are not considered.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2" specific-use="star"><caption><p id="d1e1907">Comparison of mean size distributions in the SAL during AER-D from
different instruments and different sizing metrics. For clarity only upper
error bounds are shown. Horizontal error bars represent maximum bin width
due to uncertainties in both bin centre and bin width.</p></caption>
            <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f02.pdf"/>

          </fig>

      <p id="d1e1916">The PCASP was calibrated before and after the campaign, and the CDP was
calibrated and cleaned before most flights during the campaign as described
in Rosenberg et al. (2012). The PCASP and CDP employ light scattering
in order to determine particle size; thus, the nominal size bins have been
adjusted for a refractive index (RI) of dust of 1.53–<inline-formula><mml:math id="M58" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.001</mml:mn><mml:mi>i</mml:mi></mml:mrow></mml:math></inline-formula>, informed by
the refractive index closure results from Sect. 2.5, using the CStoDConverter software
(Rosenberg et al., 2012). This results in an increase in diameter of
the largest size bins due to the more absorbing imaginary part of the
refractive index as compared to PSL (polystyrene latex) used in the
manufacturer's calibrations. The software also provides uncertainties in the
bin centres and bin widths due to oscillations in the Mie scattering curve,
which can cause ambiguities in the scattering–size relationship. This
propagation of errors allows us to utilize data from the full size range
while still maintaining a measure of the sizing uncertainty and can be seen
by horizontal error bars in Fig. 2. The larger
errors around diameters of 3.5 and 20 <inline-formula><mml:math id="M59" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, for example, relate to
inflection points on the Mie scattering curves. These horizontal sizing
errors are propagated through to calculations of number and volume size
distribution errors. The first size bins are removed for both the PCASP and
CDP since the lower edges are not well defined.</p>
      <p id="d1e1936">In a similar manner to Fennec, custom bin widths were set for the CDP. The
smallest bin of the CDP was set much wider than standard, with a lower
minimum detection threshold in order to increase sensitivity to smaller
particles, and subsequent processing of the particle-by-particle data
allowed the smallest size bin to be split into four sub-bins. As a result, the
bin sizes of the CDP increase due to the refractive index correction, but
the size resolution at the small end of the spectrum is retained due to the
custom bin specifications. This prevents too much of a gap developing
between the PCASP and CDP size ranges, with the first four size bins covering
3.36–3.87, 3.76–4.18, 4.35–4.81 and 4.74–5.36 <inline-formula><mml:math id="M60" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Note that the bin
sizes overlap due to the method used to determine bin edges in
CStoDConverter.</p>
      <?pagebreak page17232?><p id="d1e1947">Bin sizes also depend on the choice of refractive index applied. In this
work, a complex refractive index (<inline-formula><mml:math id="M61" display="inline"><mml:mrow><mml:msup><mml:mi>n</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi>m</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup><mml:mo>-</mml:mo><mml:mi>i</mml:mi><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>) of
1.53–<inline-formula><mml:math id="M62" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.001</mml:mn><mml:mi>i</mml:mi></mml:mrow></mml:math></inline-formula> was used to determine the PCASP and CDP bin sizes, as determined
from Sect. 2.5, for 550 nm. Since the PCASP and
CDP operate at wavelengths of 633 and 658 nm, we assume a constant
refractive index across these wavelengths. This is supported by the
relatively flat spectral refractive index shape at these wavelengths
indicated in Fig. S2. As additional sensitivity tests, size distributions
were also computed using a real part, <inline-formula><mml:math id="M63" display="inline"><mml:mrow><mml:msup><mml:mi>m</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>, of 1.48 and 1.58
(<inline-formula><mml:math id="M64" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.53</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.05</mml:mn></mml:mrow></mml:math></inline-formula>) and imaginary parts, <inline-formula><mml:math id="M65" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>, of 0.002, 0.003 and
0.006. Particle sizes determined from the PCASP and CDP represent optically
equivalent diameters. Sensitivity in effective diameter (<inline-formula><mml:math id="M66" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) to these
changes from <inline-formula><mml:math id="M67" display="inline"><mml:mrow><mml:msup><mml:mi>m</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> were less than 0.2 <inline-formula><mml:math id="M68" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (&lt; 5 %),
and those from changes in <inline-formula><mml:math id="M69" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> were less than 0.9 <inline-formula><mml:math id="M70" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (&lt; 20 %).
However, within the likely range of <inline-formula><mml:math id="M71" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> (0.001–0.002) as derived in
Sect. 2.5, changes in <inline-formula><mml:math id="M72" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> were &lt; 0.1 <inline-formula><mml:math id="M73" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (&lt; 3 %). Therefore, we consider the uncertainty in
<inline-formula><mml:math id="M74" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> to refractive index to be a maximum of 5 % reflecting the
uncertainty due to likely values of both <inline-formula><mml:math id="M75" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M76" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula>.</p>
      <p id="d1e2125">The OAPs (CIP15, CIP100, 2-DS) measure particles in two
perpendicular directions: the first aligned with the photodiode array (<inline-formula><mml:math id="M77" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula>)
and the second along the direction of aircraft motion (<inline-formula><mml:math id="M78" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula>). This provides a
two-dimensional projection of a particle (McFarquhar et al., 2017).
Although the OAPs do not require assumptions about refractive index to
derive size, they can be subject to several systematic uncertainties
associated with the processing/sizing method (McFarquhar et al., 2017). Thus, to investigate some of these uncertainties, the 2-DS data were processed
in two different ways, using two different sizing metrics.</p>
      <p id="d1e2142">Firstly, data from all three OAPs were processed using the System for OAP
Data Analysis (SODA-2) developed at NCAR. The SODA-2 removes out-of-focus
images and various instrument artefacts including accounting for a stuck
diode in the middle of the CIP-100 array. An “all-in” method was applied
where particles are only counted when they fall completely within the
photodiode array. The particle size was defined as the diameter of the
smallest circle enclosing the particle (denoted “CC” – circumscribing
circle) and thus for non-spherical particles may lead to an overestimation of particle size. Secondly, data from the 2-DS instrument were analysed using
the Optical Array Shadow Imaging Software (OASIS), developed by the National
Centre for Atmospheric Science (NCAS) and Droplet Measurement Technologies. Particle sizes were
calculated using the mean of the <inline-formula><mml:math id="M79" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M80" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> dimensions of each particle image
(denoted “XY”) using a “centre-in” method where particles are only counted
when the centre of the particle falls completely within the photodiode
array. The <inline-formula><mml:math id="M81" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M82" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> dimensions are measured along the probe array; i.e. the
particle is not rotated to minimize or maximize either dimension.</p>
      <p id="d1e2173">The mean XY method is considered to give a more representative diameter for
non-spherical particles than the CC metric. Area-equivalent diameters were
not calculated because particles can sometimes appear hollow on the OAPs
(McFarquhar et al., 2017), which would lead to undersizing. If the
particle image is an ellipse, the mean XY diameter will be larger than an
ellipse area-equivalent diameter, as used by the filter sample analysis for
example. However, the OAP images capture 2-D image projections of the
particles in their atmospheric orientation, while the filter samples will be collected with their largest surface lying parallel to the filter
sample and therefore may be oversized in this context.<?pagebreak page17233?> An additional
motivation for testing this second processing option for the 2-DS was for
comparison with Fennec data (Ryder et al., 2013b) which were processed using
an all-in, mean XY method for the CIP15.</p>
      <p id="d1e2176">Since particles detected by the 2-DS during AER-D mostly cover one to seven pixels,
the impact of centre-in versus all-in is considered small. The sample area
is adjusted for the effective array width, which is different depending on
whether all-in or centre-in is used (McFarquhar et al., 2017), and
therefore the calculated number concentrations account for this. The sizing
metric (i.e. XY versus CC) has the greatest impact on the final size
distribution. Smallest and largest size bins were removed for the OAP data,
and data were excluded for size bins in SLRs where fewer than four particles
were detected as an additional measure for removing noise (equating to
number concentrations of around 10<inline-formula><mml:math id="M83" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> cm<inline-formula><mml:math id="M84" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for the 2-DS and CIP15 for
typical sampling times of around 20 min or 132 km on the BAe 146). The
CIP100 suffered from noise and did not detect any particles within its size
range (<inline-formula><mml:math id="M85" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 200 <inline-formula><mml:math id="M86" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m following exclusion of the first size
bin).</p>
      <p id="d1e2217">Uncertainties in number concentration for all size probes are propagated
from 1Hz measurements, through to means over SLRs, through to the AER-D
campaign averages. For all probes, random errors (due to counting and
discretization error) and systematic errors (due to sample area uncertainty
and bin size centre and width from Mie singularities) were accounted for in
their contribution to total number concentration errors, and propagated by
standard analytical error propagation. That is, random error can be minimized by
increasing the sample size (averaging across the campaign), while systematic
error remains constant. For the CDP at <inline-formula><mml:math id="M87" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 20 <inline-formula><mml:math id="M88" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, bin size
uncertainty was found to dominate the total uncertainty in dN/dlogD and
dV/dlogD. Horizontal error bars in Fig. 2
represent the maximum uncertainty in bin edges, derived from uncertainties
in both bin centre and bin width. Uncertainties in bin size contribute to
uncertainties in both dN/dlogD and dV/dlogD, and therefore the relative
uncertainties do not change significantly between the two panels. All error
bars represent maximum uncertainty.</p>
      <p id="d1e2235">Figure 2 shows an instrument comparison for the
five instruments for the mean size distribution in the SAL. It can be seen
that the CIP15 and 2-DS cover similar size ranges, and the CDP overlaps both
of these instruments at the smallest size bins. However, different number
concentrations are detected by the CIP15 and 2-DS, which becomes more evident
as size approaches 100 <inline-formula><mml:math id="M89" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Greater number and volume distributions
are seen from the CIP15 than the 2-DS, although when the same processing and
sizing assumptions are used (CIP15 CC, blue, and 2-DS CC, orange), the size
distributions agree within error bars. The 2-DS XY processing (green) results
in a lower number distribution and a smaller maximum size, as expected for
non-spherical dust particles (Sect. 3.2) because
the CC metric will oversize a non-spherical particle. Therefore, several
choices are made in terms of how best to use data from each instrument in
the analysis of size distributions and subsequent optical properties, as
follows. We use the full size range of the PCASP for the accumulation mode,
for the coarse mode the CDP is used up to 20 <inline-formula><mml:math id="M90" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, and the giant mode
is taken from the 2-DS XY processing and metric since this is a better metric
for non-spherical dust particles and also consistent with the Fennec data
processing. This size distribution is referred to as “FULL PSD”.</p>
      <p id="d1e2252">Size distributions are summarized with commonly used metrics of effective
diameter, <inline-formula><mml:math id="M91" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, (Hansen and Travis, 1974) (sometimes known as
the volume-surface diameter; Hinds, 1999), and volume median diameter
(VMD, the diameter below which half of the volume size distribution lies;
Seinfeld and Pandis, 2006). Additionally, we present the maximum
size detected, <inline-formula><mml:math id="M92" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, by the 2-DS XY as a useful metric of the largest
size present in the atmosphere. Weinzierl et al. (2009, 2011) present
maximum size measured at a concentration above 10<inline-formula><mml:math id="M93" 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> cm<inline-formula><mml:math id="M94" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. Here we
choose to simply present the maximum particle size detected, since the
number concentration detected depends on the width of the size bin employed
by the particular instrument operated and is not directly comparable. The
sizing instruments operated during AER-D do not have a minimum detection
concentration level, but at low particle concentrations the sampling
statistics simply become poor, introducing an effective detection limit. Therefore, we remove cases where fewer than four particles are detected over an SLR as previously mentioned, with an implicit effect of removing data where
concentrations are lower than 10<inline-formula><mml:math id="M95" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> cm<inline-formula><mml:math id="M96" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for the 2-DS and CIP15.</p>
      <p id="d1e2326">Some CIP15 AER-D data were also processed using a centre-in, mean XY metric,
but unfortunately it was not possible to process data for all the SLRs with
this method. Therefore, these data were used to provide information on instrumental
differences between the 2-DS and CIP15 when processed with the same size
metric (XY mean). It was found that the impact on the FULL particle size distribution (PSD) was very
small (<inline-formula><mml:math id="M97" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> differed by under 1 %), but that <inline-formula><mml:math id="M98" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> was up to
6 % larger with the CIP15 XY compared to the 2-DS XY. The upper uncertainty
of 6 % in <inline-formula><mml:math id="M99" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> was therefore propagated in combination with the other
uncertainties in <inline-formula><mml:math id="M100" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>.</p>
</sec>
<sec id="Ch1.S2.SS3.SSS3">
  <title>Size distribution behind Rosemount inlets</title>
      <p id="d1e2379">In addition to the main size distribution combination described above, a
further size distribution is calculated in order to represent the size
distribution reaching the nephelometer and PSAP, accounting for inlet
enhancements and losses as well as pipe losses (Trembath, 2012; Ryder et
al., 2013b). In order to do this, the FULL PSD is adjusted for the
size-resolved, height-dependent loss or enhancement as shown in
Fig. S1. Since particles larger than 5 <inline-formula><mml:math id="M101" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter do not reach the
nephelometer or PSAP, the choice of instrument at sizes larger than this is
irrelevant. There is a net loss of particles at <inline-formula><mml:math id="M102" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 2–3 <inline-formula><mml:math id="M103" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
and an enhancement of the number of particles in the accumulation mode at
<inline-formula><mml:math id="M104" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 2–3 <inline-formula><mml:math id="M105" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. We term<?pagebreak page17234?> this size distribution “ACC PSD” since it
predominantly represents the accumulation mode.</p>
</sec>
<sec id="Ch1.S2.SS3.SSS4">
  <title>Filter sample collection</title>
      <p id="d1e2424">Aerosol filter samples were collected using the FAAM airborne filter
collection system (Andreae et al., 2000; Formenti et al., 2008; McConnell
et al., 2010) behind a separate inlet dedicated to filter samples (i.e.
different to the Rosemount inlets). This is the same inlet used to collect
ice nuclei particle samples presented in Price et al. (2018), in many
cases samples were collected in parallel. The inlet passing efficiency has
not been formally determined, though Andreae et al. (2000)
found that while mounted on the previous C-130 aircraft, the same filter inlet restricted measurements to 35 % of the coarse-mode mass (defined as
<inline-formula><mml:math id="M106" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 1.4 <inline-formula><mml:math id="M107" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) in sea salt aerosol compared to ground-based
observations. Further details are available in Price et al. (2018).</p>
      <p id="d1e2441">Aerosol particles were sampled by filtration onto a stacked-filter unit
(SFU) with three stages, though only one stage was used in AER-D. Aerosols
were collected on 47 mm diameter nucleopore filters with pore sizes of 0.2 or
0.4 <inline-formula><mml:math id="M108" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m using either a standard plastic filter holder as used
previously (e.g. Formenti et al., 2008) or on a newly developed adjusted
plastic filter holder with a lip on the edge removed for ease of loading.
Depending on the holder and pore size used, different support grids were
used – either plastic, Millipore fine mesh metal or JSHoldings coarse mesh
metal. In total 22 filter samples were collected during AER-D flights,
although problems were encountered with many samples ranging from
difficulties mounting and removing the support grids into the old filter
holder, very low flow rates when combining the 0.2 <inline-formula><mml:math id="M109" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m nucleopore pore
sizes and Millipore grid, and unexplained silicon contamination on some
samples. As a result, many of the filter samples did not display the
expected number of particles upon laboratory analysis. Therefore, we were
forced to discard many samples, and four samples of the best data were
analysed for size, shape and chemical composition: two SLRs in the
MBL (b920 R2, b928 R2) and two SLRs in the SAL (b920 R5, b932 R6). This was done in order to
give a snapshot of these properties during AER-D.</p>
</sec>
</sec>
<sec id="Ch1.S2.SS4">
  <title>Filter sample analysis</title>
      <p id="d1e2465">Filter samples were analysed by scanning electron microscopy (SEM,
instrument model JEOL JSM 6301F) coupled to an X-ray energy-dispersive
spectrometer (Silicon Drift X-Max 80 mm<inline-formula><mml:math id="M110" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> Detector and Aztec
Advanced-INCA350 analyzer, Oxford Instruments) to provide information on the
coarse and fine fractions respectively. Analysis was performed on a portion
of filter cut and mounted on an aluminum stub using a double-sided adhesive
and then covered with a thin film of platinum (Pt) by sputter coating (Jeol
JFC 1100E). Particles were found to be evenly distributed across the filter
sample. Images were acquired by a series of transects at two magnifications
(<inline-formula><mml:math id="M111" display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">2000</mml:mn></mml:mrow></mml:math></inline-formula> (55.9 nm pixel<inline-formula><mml:math id="M112" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) and <inline-formula><mml:math id="M113" display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">10</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">000</mml:mn></mml:mrow></mml:math></inline-formula> (11.0 nm pixel<inline-formula><mml:math id="M114" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>)),
scanning between 397  and 1116 particles per sample.</p>
      <p id="d1e2524">Particles were sized by processing the SEM images, which are essentially 2-D
projections of 3-D particles. The 2-D projections were fitted with a
circumscribed ellipse, to produce an ellipse area-equivalent diameter, where
the major and minor axes (<inline-formula><mml:math id="M115" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M116" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">min</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) are used to define the
particle diameter <inline-formula><mml:math id="M117" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> according to <inline-formula><mml:math id="M118" display="inline"><mml:mrow><mml:mi>d</mml:mi><mml:mo>=</mml:mo><mml:mo>(</mml:mo><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">min</mml:mi></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>/</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. The
aspect ratio was accordingly calculated using <inline-formula><mml:math id="M119" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">min</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>.</p>
      <p id="d1e2606">It was not possible to use automated image contrast to calculate projected
particle area because of a high degree of variability in particle contrast.
Our filters sizing this technique may oversize the particle size for two
reasons. Firstly, the area of a fitted ellipse may be larger than a
projected particle area, though the particles were not noticeably jagged
around their edges. Secondly, our method may oversize particle volume where
the shape is a platy silicate and has a tendency to fall with its largest
surface parallel to the substrate. For example, Chou et al. (2008) found the height of dust particles examined under SEM to be around
one-third of their major axis length. Additionally, we tested the
sensitivity of the filters PSD to using the mean XY and CC sizing methods
applied to the OAP data (not shown). Using a mean XY method on the filter data did not produce significantly different results, while using the CC
method was found to shift the PSD towards larger particles, similar to the
findings from the OAP size metric comparisons.</p>
      <p id="d1e2609">Semi-quantitative elemental chemical analyses integrate the following
elements: Na, Mg, Al, Si, P, S, Cl, K, Ca, Ti, Mn and Fe. The results are
expressed as a weight percentage of the associated oxides (<inline-formula><mml:math id="M120" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">Na</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>, MgO,
<inline-formula><mml:math id="M121" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">Al</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M122" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SiO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M123" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">P</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">5</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M124" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, Cl, <inline-formula><mml:math id="M125" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">K</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>, CaO,
<inline-formula><mml:math id="M126" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">TiO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, MnO, <inline-formula><mml:math id="M127" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">Fe</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) normalized to 100 %. The composition type
of each particle is then identified based on these percentages as belonging to one of
the following categories: alumino-silicates, quartz, sulfate, salt,
thenardite, gypsum, Ca-rich, Ti-rich, Fe-rich and others. These are
interpretations based on the elementary chemical analysis. For example, if we
observe the simultaneous presence of calcium and sulfur (typically within
10 % of one another), this could be several possible minerals: anhydrite
(<inline-formula><mml:math id="M128" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CaSO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>), bassanite (<inline-formula><mml:math id="M129" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CaSO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M130" display="inline"><mml:mo>⋅</mml:mo></mml:math></inline-formula> 0.5(<inline-formula><mml:math id="M131" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>)) and gypsum
(<inline-formula><mml:math id="M132" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CaSO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M133" display="inline"><mml:mrow class="chem"><mml:mn mathvariant="normal">2</mml:mn><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>), though the most probable atmospheric form is
gypsum. Sulfate is classified by the dominance of <inline-formula><mml:math id="M134" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. Thenardite is
classified when both <inline-formula><mml:math id="M135" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">Na</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M136" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> are dominant. Salt is classified
by percentages of both <inline-formula><mml:math id="M137" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">Na</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula> and Cl being high, indicating halite
particles of marine origin. Alumino-silicates, quartz, thenardite, gypsum
and Fe-rich particles indicate terrigenous particles in these cases. Only
one black carbon chain-like structure was observed during the analysis of
over 6500 particles, and therefore this aerosol category is not included.</p>
      <p id="d1e2839">Although particles may frequently be a mix of several composition types,
they were classified according to their component type which made up the
greatest oxide<?pagebreak page17235?> percentage. This may be a particularly important assumption
regarding the iron component, which was consistently present in small
amounts on most particle types but only classified as iron when iron was the
dominant component; i.e. in general when iron oxide constituted over 50 %
of the composition. More complex methods of accounting for iron as a minor
component are possible (e.g. Kandler et al., 2011a; Balkanski et al., 2007) but are beyond the scope of this work. Although composition
information is available for all particles sampled under magnifications of
<inline-formula><mml:math id="M138" display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">2000</mml:mn></mml:mrow></mml:math></inline-formula>, many particles sampled under the high magnification did
not provide a strong enough signal to provide composition data. Thus, the
number of particles available for composition analysis in the fine fraction
is much lower than that for the coarse fraction.</p>
      <p id="d1e2852">Filter sample analyses use subsets of data from each magnification in order
to take advantage of the best counting statistics for each size range and
optimal viewing at each magnification. Filter sample size distributions are
calculated using fairly finely resolved size bins from 0.05 to 40 <inline-formula><mml:math id="M139" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
as shown in Fig. 7. However, at each
magnification, sensitivity to the smallest particles detected is low due to
a low SEM signal (fewer photons emitted for smaller volume particles). Therefore, particles smaller than 0.1 and 0.5 <inline-formula><mml:math id="M140" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m are excluded for
<inline-formula><mml:math id="M141" display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">2000</mml:mn></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M142" display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">10</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">000</mml:mn></mml:mrow></mml:math></inline-formula> respectively. Additionally, for the
<inline-formula><mml:math id="M143" display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">10</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">000</mml:mn></mml:mrow></mml:math></inline-formula> magnification, not many particles larger than 1 <inline-formula><mml:math id="M144" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
are counted in comparison to <inline-formula><mml:math id="M145" display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">2000</mml:mn></mml:mrow></mml:math></inline-formula>, so particles larger than 1 <inline-formula><mml:math id="M146" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m are also excluded.</p>
      <p id="d1e2930">For aspect ratio, composition and refractive index analyses, particles sized
0.1 to 0.5 <inline-formula><mml:math id="M147" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m are taken from the <inline-formula><mml:math id="M148" display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">10</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">000</mml:mn></mml:mrow></mml:math></inline-formula> magnification,
while particles sized between 0.5 and 40 <inline-formula><mml:math id="M149" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m are taken from the
<inline-formula><mml:math id="M150" display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">2000</mml:mn></mml:mrow></mml:math></inline-formula> magnification and scaled appropriately to account for the
different substrate areas examined under the different magnifications. Size-resolved composition data utilizes six size bins with edges at 0.1, 0.5,
1.0, 2.5, 5, 10 and 40 <inline-formula><mml:math id="M151" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Information for the full filters size
distribution accordingly covers 0.1 to 40 <inline-formula><mml:math id="M152" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Additionally, bulk
filter sample properties are calculated specifically for the accumulation
mode, covering diameters 0.1 to 2.5 <inline-formula><mml:math id="M153" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, in order to replicate the
in-cabin measurements behind the Rosemount inlets and also for the bulk
sample from 0.1 to 40 <inline-formula><mml:math id="M154" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m to cover the full size distribution. Aspect
ratios are presented as number fractions; composition is presented as volume
fraction.</p>
</sec>
<sec id="Ch1.S2.SS5">
  <title>Derivation of refractive index</title>
<sec id="Ch1.S2.SS5.SSS1">
  <title>Refractive index iterated from optical and size measurements</title>
      <p id="d1e3011">In order to determine the accumulation mode refractive index for each
individual SLR, measurements of scattering and absorption from the
nephelometer and PSAP are used in combination with Mie scattering code,
taking input from the measured size distributions. Since the nephelometer
and PSAP only measure scattering and absorption from the accumulation mode
due to inlet effects, the refractive indices derived only represent the
accumulation mode up to 2.5 <inline-formula><mml:math id="M155" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and not the coarse mode. The method
is identical to that described in Ryder et al. (2013b): a Mie scattering
code is used to generate optical properties at 550 nm, using the ACC PSD,
with refractive index of <inline-formula><mml:math id="M156" display="inline"><mml:mrow><mml:msup><mml:mi>m</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1.53</mml:mn></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M157" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> incrementing in
steps of 0.0005 from 0.0005 to 0.006 but with an additional smallest value
of 0.0001 which was required for the MBL SLRs. The value of <inline-formula><mml:math id="M158" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> which
produced best agreement with the SSA from the nephelometer and PSAP was
selected for each SLR. The resulting values of <inline-formula><mml:math id="M159" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> are shown in
Fig. 3, with modal values of 0.001i for SAL SLRs
and <inline-formula><mml:math id="M160" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.0001</mml:mn><mml:mi>i</mml:mi></mml:mrow></mml:math></inline-formula> for MBL SLRs. This set of refractive index data is referred to
hereafter as the “iterated refractive indices”.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><caption><p id="d1e3082">Histogram of derived imaginary part of the refractive index at 550 nm (<inline-formula><mml:math id="M161" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>) from iterations for the accumulation mode, shown separately
for SLRs in the SAL and MBL.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f03.pdf"/>

          </fig>

      <p id="d1e3102">The derived iterated refractive indices were then used in two ways. Firstly,
a value of 1.53–<inline-formula><mml:math id="M162" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.001</mml:mn><mml:mi>i</mml:mi></mml:mrow></mml:math></inline-formula> was used to correct all size distributions from the
PCASP and CDP. Secondly, iterated refractive indices derived for each SLR
were selected to generate optical properties for the FULL PSD and ACC PSD
described in Sect. 2.6.</p>
</sec>
<sec id="Ch1.S2.SS5.SSS2">
  <title>Refractive index from filter samples</title>
      <p id="d1e3121">We use the composition volume fraction and spectral refractive index data of
seven aerosol/mineral components in order to compute refractive indices. These
are alumino-silicates, quartz, carbonates, gypsum, iron-rich ones, sodium
chloride (sea salt) and sulfate-rich ones. Alumino-silicate is represented by a
mean of illite and kaolinite refractive indices, carbonates by calcite
refractive indices, and iron-rich refractive indices by a mean of hematite and goethite
refractive indices.<?pagebreak page17236?> Sea salt is represented with NaCl refractive indices.
The sulfate-rich category is represented by ammonium sulfate refractive
indices, assumed to be the most likely atmospheric composition. Thenardite
is also included in the sulfate-rich category as no refractive index data
are available for it, similar to Kandler et al. (2009). Literature data were taken as follows: illite (Egan and Hilgeman, 1979; Querry,
1987), kaolinite (Egan and Hilgeman, 1979; Glotch et al., 2007), quartz
(Shettle and Fenn, 1979; Peterson and Weinman, 1969), calcite
(Querry et al., 1978; Long et al., 1993), gypsum (Long et
al., 1993), hematite (Shettle and Fenn, 1979; Bedidi and Cervelle, 1993;
Marra et al., 2005), goethite (Bedidi and Cervelle, 1993; Glotch and
Rossman, 2009), sodium chloride (Toon et al., 1976) and ammonium
sulfate (Toon et al., 1976). Where no spectral data are
available, values are linearly interpolated across wavelengths. Refractive
indices are then calculated by weighting each mineral component by its
volume fraction given from the composition analysis in Sect. 2.4, a method which assumes that particles are
internally, homogenously mixed. Although it was evident from the SEM
analysis that the particles are externally mixed, and it is known that
internal and external mixing can result in different optical properties
(McConnell et al., 2010), we employ this method partly for simplicity and
partly for consistency with previous work (e.g. Kandler et al., 2009,
2011a; Klaver et al., 2011; Formenti et al., 2014). These refractive
indices are then used with the size distribution data from the wing probes
to generate optical properties using Mie scattering code.</p>
</sec>
</sec>
<sec id="Ch1.S2.SS6">
  <title>Calculation of optical properties</title>
      <p id="d1e3131">Optical properties (SSA, MEC and <inline-formula><mml:math id="M163" display="inline"><mml:mi>g</mml:mi></mml:math></inline-formula>) are calculated using a Mie scattering
code, where dust particles are assumed to be spheres. Size distributions
used are taken from the wing probes, representing either the FULL PSD or the
ACC PSD. Refractive indices are taken from either the iterated RI method
(Sect. 2.5.1) or from internal or external mixing
RI values calculated from the filter samples (Sect. 2.5.2).</p>
      <p id="d1e3141">When the iterated RI values are used, composition, and therefore <inline-formula><mml:math id="M164" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>,
is assumed to remain constant with particle size. This allows the iterated
RI for the accumulation mode to be applied to the full size distribution.
For all cases <inline-formula><mml:math id="M165" display="inline"><mml:mrow><mml:msup><mml:mi>m</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> was assumed to be 1.53. Iterated values of
<inline-formula><mml:math id="M166" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> specific to each SLR were used. For the MBL <inline-formula><mml:math id="M167" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> varied
between 0.0001 and 0.0005, and for the SAL <inline-formula><mml:math id="M168" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> varied between 0.0005
and 0.0025 (as shown in Fig. 3). Although a value of
1.53 for <inline-formula><mml:math id="M169" display="inline"><mml:mrow><mml:msup><mml:mi>m</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> is higher than that produced by the filter sample
composition results (Sect. 3.5, 1.47–1.49) the
filter result is likely biased low due to the reasons discussed in Sect. 3.5. We also performed a sensitivity test to using
<inline-formula><mml:math id="M170" display="inline"><mml:mrow><mml:msup><mml:mi>m</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> of 1.48 and 1.58 and found that <inline-formula><mml:math id="M171" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> changed by up to
5 % and SSA by under 1 %.</p>
      <p id="d1e3233">Where composition from filter samples is used, RI is allowed to vary as a
function of particle size according to the composition results. For internal
mixing assumptions, the refractive indices calculated according to Sect. 2.5.2 are used. For external mixing assumptions,
size distributions of each mineral component are calculated by weighting the
size distribution from the wing probes for each mineral component using its
number fraction. Scattering properties for the size distribution of each
mineral are then computed using Mie scattering code and the same literature
refractive indices as described above. Summing scattering and absorption
over all minerals then provides the total optical properties for the
external mixing case.</p>
      <p id="d1e3236">Although it is clear that dust particles are not spherical, sensitivity of
SSA to shape was tested by Otto et al. (2009) and Johnson and
Osborne (2011), who found that SSA changed by under 1 % and 2 %
respectively when non-spherical particles were assumed. This is less than
our uncertainty in SSA of 5 % given above due to the refractive index, and
therefore we consider this an acceptable assumption.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T4" specific-use="star"><caption><p id="d1e3243">Details of dust uplift events determined from SEVIRI RGB imagery
driving dust sampled by the aircraft. Uplift numbers correspond to primary,
secondary or tertiary uplift, also indicated in
Fig. 1.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="7">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="right"/>
     <oasis:thead>
       <oasis:row>
         <oasis:entry colname="col1">Flight</oasis:entry>
         <oasis:entry colname="col2">Uplift</oasis:entry>
         <oasis:entry colname="col3">Event driving uplift</oasis:entry>
         <oasis:entry colname="col4">Time and date of uplift</oasis:entry>
         <oasis:entry colname="col5">Uplift longitude</oasis:entry>
         <oasis:entry colname="col6">Uplift latitude</oasis:entry>
         <oasis:entry colname="col7">Age at aircraft</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">number</oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5">centre</oasis:entry>
         <oasis:entry colname="col6">centre</oasis:entry>
         <oasis:entry colname="col7">sampling, days</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">b920</oasis:entry>
         <oasis:entry colname="col2">n/a</oasis:entry>
         <oasis:entry colname="col3">MCS and haboob</oasis:entry>
         <oasis:entry colname="col4">2 Aug 15:00 to</oasis:entry>
         <oasis:entry colname="col5">3.0</oasis:entry>
         <oasis:entry colname="col6">23.5</oasis:entry>
         <oasis:entry colname="col7">3.9 to 4.6</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">3 Aug 07:00</oasis:entry>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">b923/b924</oasis:entry>
         <oasis:entry colname="col2">n/a</oasis:entry>
         <oasis:entry colname="col3">MCS and haboob</oasis:entry>
         <oasis:entry colname="col4">10 Aug 10:00 to</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M172" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6">21.0</oasis:entry>
         <oasis:entry colname="col7">1.9 to 2.2</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">10 Aug 19:00</oasis:entry>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">b928</oasis:entry>
         <oasis:entry colname="col2">1</oasis:entry>
         <oasis:entry colname="col3">Convection under widespread</oasis:entry>
         <oasis:entry colname="col4">13 Aug 12:00 to</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M173" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">8.5</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6">23.0</oasis:entry>
         <oasis:entry colname="col7">2.2 to 3.1</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">patchy cloud</oasis:entry>
         <oasis:entry colname="col4">14 Aug 10:00</oasis:entry>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">2</oasis:entry>
         <oasis:entry colname="col3">MCS and haboob</oasis:entry>
         <oasis:entry colname="col4">14 Aug 19:00 to</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M174" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2.2</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6">20.4</oasis:entry>
         <oasis:entry colname="col7">1.4 to 1.8</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">15 Aug 05:00</oasis:entry>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">b932</oasis:entry>
         <oasis:entry colname="col2">1</oasis:entry>
         <oasis:entry colname="col3">MCS and haboob</oasis:entry>
         <oasis:entry colname="col4">17 Aug 10:00 to</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M175" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1.5</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6">21.5</oasis:entry>
         <oasis:entry colname="col7">2.4 to 3.0</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">18 Aug 01:00</oasis:entry>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">2</oasis:entry>
         <oasis:entry colname="col3">Small-scale local</oasis:entry>
         <oasis:entry colname="col4">18 Aug 12:00 to</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M176" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">5.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6">24.5</oasis:entry>
         <oasis:entry colname="col7">1.9 to 2.0</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">convection</oasis:entry>
         <oasis:entry colname="col4">18 Aug 14:00</oasis:entry>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">b934</oasis:entry>
         <oasis:entry colname="col2">1</oasis:entry>
         <oasis:entry colname="col3">Small-scale convection</oasis:entry>
         <oasis:entry colname="col4">22 Aug 21:00 to</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M177" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1.3</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6">22.5</oasis:entry>
         <oasis:entry colname="col7">2.6 to 2.9</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">and haboob</oasis:entry>
         <oasis:entry colname="col4">23 Aug 03:00</oasis:entry>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">2</oasis:entry>
         <oasis:entry colname="col3">Small-scale convection</oasis:entry>
         <oasis:entry colname="col4">23 Aug 22:00 to</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M178" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">6.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6">20.0</oasis:entry>
         <oasis:entry colname="col7">1.6 to 1.7</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">and haboob</oasis:entry>
         <oasis:entry colname="col4">24 Aug 01:00</oasis:entry>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">3</oasis:entry>
         <oasis:entry colname="col3">Small-scale convection</oasis:entry>
         <oasis:entry colname="col4">24 Aug 20:00 to</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M179" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">13.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6">19.5</oasis:entry>
         <oasis:entry colname="col7">0.7 to 0.8</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">and haboob</oasis:entry>
         <oasis:entry colname="col4">24 Aug 23:00</oasis:entry>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"/>
         <oasis:entry colname="col7"/>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

</sec>
</sec>
<sec id="Ch1.S3">
  <title>Results</title>
<sec id="Ch1.S3.SS1">
  <title>Dust sources and vertical structure</title>
      <p id="d1e3795">Figure 1 shows the dust uplift locations (sources)
determined using SEVIRI RGB imagery for dust sampled during each AER-D
flight. Table 4 shows the corresponding
meteorological event driving the uplift and also the age of dust when
sampled by the aircraft. Dust sampled by the first two flights, b920 and
b923/924 originated from large-scale dust events uplifted in easily
identifiable single events. The b920 dust was uplifted over southern Algeria
(blue circle in Fig. 1) and subsequently
transported northwards and then westwards. The dust emerged over the
Atlantic from southern Morocco, being sampled by the aircraft after around 4 days' transport. The b923/b924 dust was uplifted further west, over northern
Mali (green oval in Fig. 1), and was also
subsequently transported northwestwards, emerging over the Atlantic over
southern Morocco and sampled by the aircraft after a shorter time of 2 days
due to the more direct transport path.</p>
      <p id="d1e3798">During the days leading up to flight b928, there was a change in the
dominant meteorological dust export mechanism, as described by Liu et al. (2018). First, dust was uplifted over northern Mauritania (orange circle
number 1) underneath widespread altocumulus cloud, which moved slowly to the
southwest. Here, it became mixed with dust which had originated from
northern Mali (orange circle number 2) where it had been uplifted by an MCS
and haboob. This moved rapidly westwards, driven by strengthened 700 mb
winds, which characterized the second phase of ICE-D (Liu et al., 2018).
The two dust events became mixed together and subsequently transported dust
over the Atlantic via the Mauritanian coastline, thus taking a more direct
southerly transport route than the dust exported and sampled by the first
two flights of the campaign (b920 and b924). Thus, the dust sampled during
b928 was a mixture of<?pagebreak page17237?> dust from two different source regions. The final two
flights, b932 and b934, consist of dust uplift events which subsequently
overpassed secondary (or tertiary) uplift events and are therefore
considered as dust from a mixture of the identified sources. The dust
sampled during b932 was initially uplifted by an MCS and haboob close to the
Mali–Algerian border, and some small-scale reinvigorated convection caused
additional uplift over northern Mali before the dust was transported
southwestwards towards the Mauritanian coastline. Dust encountered during
b934 was also initially uplifted in almost the same region along the
Mali–Algeria border by an MCS and haboob, and on each subsequent evening a
new convective cell developed over the transported dust with a new haboob: over the Mali–Mauritanian border (purple circle number 2) and then over
western Mauritania (purple circle number 3). Therefore, the range of possible
dust ages for b934 is very large (16 h to 3 days). The range of sources
identified during AER-D is consistent with well-known source regions in the
literature (Engelstaedter et al., 2006; Formenti et al., 2011; Evan et
al., 2016; Scheuvens et al., 2013), particularly the Mali–Algeria border
hotspot downwind of the gap between the Atlas and Ahaggar Mountains
(Potential Source Area 3 in Formenti et al., 2011), which contributed to
four of the five AER-D dust events.</p>
      <p id="d1e3801">Figure 4 shows the vertical structure of the five
dust events sampled during AER-D from in situ aircraft measurements. Four
events (b920, b928, b932 and b934) display typical SAL structure, with
elevated dust from a base of between 0.5 and 1.5 km up to an upper bound of 5 km (6 km in one case) overlying the MBL. Accumulation mode extinction
coefficients vary from around 100 to 500 Mm<inline-formula><mml:math id="M180" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in this layer, sometimes
with fairly constant values in the vertical (b920, b934). Other layers
were more sinuous (b932, b928) but always had accumulation mode scattering
Ångström exponents (SAE; 700 to 450 nm) of a fairly constant value around
<inline-formula><mml:math id="M181" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn></mml:mrow></mml:math></inline-formula>
– a clear indication of coarser particles. Within the SAL, water vapour
mixing ratios were low (under 10 g kg<inline-formula><mml:math id="M182" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) and potential temperature increased
slowly with altitude. Relative humidities were low at 30 %–50 % at altitudes
where SLRs were performed. Contrastingly, in the MBL relative humidities
were high (&gt; 90 %) as expected, with the MBL capped by a
temperature inversion. SAE values in the MBL were variable, sometimes
exhibiting a jump to positive values (b920, b934) suggesting a dominance of
smaller particles, whereas sometimes hardly displaying any difference to the
overlying dust (b928, b932). In the former two cases, the PCASP size
distribution confirms a greater relative contribution from fine (<inline-formula><mml:math id="M183" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 0.3 <inline-formula><mml:math id="M184" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) particles in comparison to those sized 0.3 to 3 <inline-formula><mml:math id="M185" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m.
This vertical structure is as expected for the region in summer and in
keeping with the elevated and dusty SAL above the MBL (Prospero and
Carlson, 1972).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><caption><p id="d1e3862">Vertical structure observed during the five flights from in situ
measurements during aircraft profiles, in the region where the SLRs were
performed. Potential temperature (K; red), water vapour mixing ratio (<inline-formula><mml:math id="M186" display="inline"><mml:mi>r</mml:mi></mml:math></inline-formula>,
g kg<inline-formula><mml:math id="M187" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, black), accumulation mode extinction (Mm<inline-formula><mml:math id="M188" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, black; note different
<inline-formula><mml:math id="M189" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula>-axis range for b924) and SAE for the
accumulation mode between 450 and 700 nm (blue). Numbers at the top right of
each panel indicate accumulation mode AOD at 550 nm.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f04.pdf"/>

        </fig>

      <p id="d1e3910">In contrast, the dust event sampled on flights b923 and b924 displays very
large dust loadings and different vertical structure. The upper SAL, from
2.5 to 5 km, displays a roughly constant potential temperature and water
vapour mixing ratio, with extinction coefficients of around 140 Mm<inline-formula><mml:math id="M190" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>.
Between 0.5 and 2.5 km, dust loadings become extremely high, reaching 2122 Mm<inline-formula><mml:math id="M191" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> at 1.2 km and contributing to the very high AOD of 2.54 for the
accumulation mode only (including coarse particles would increase the
estimated AOD further). To the authors' knowledge, this is the highest
aircraft-measured value of dust-related extinction measured for dust
transported over the ocean, and it is explored further by Marenco
et al. (2018). (Note that lidar-derived AODs and extinction shown
by (Marenco et al., 2018) are slightly lower than
those shown here, which may be due to different extinction properties of the
dust at the lidar wavelength of 355 nm, the Rosemount inlet enhancement
effects shown in Fig. S2, or the differences between a lidar curtain and
sloped aircraft in situ profile.) Moisture levels here decrease with
decreasing altitude (8–12 g kg<inline-formula><mml:math id="M192" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) and are larger than observed within
dust during the other flights. The higher levels of moisture are perhaps not
surprising given that an MCS haboob uplifted this dust 2 days earlier, and
1 day earlier Saharan boundary layer (SABL) convection can be seen
impacting the dust over northern Mauritania (consistent with Marsham et al., 2013; and recycling of moisture
within the dusty SABL in Ryder et al., 2015). Note that these<?pagebreak page17239?> values of extinction do not include the coarse
mode, and therefore actual extinction values will be even higher. Beneath
the thick, low-altitude dust layer was a shallow MBL extending up to 500 m.
This unusual vertical structure of intense, thick dust within the bottom
half of the SAL is not in keeping with the conventional SAL model
(Prospero and Carlson, 1972) of well-mixed elevated dust throughout
the whole SAL and is therefore of additional interest. This is discussed in
detail by Marenco et al. (2018).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><caption><p id="d1e3951">Size distributions for SLRs <bold>(a)</bold> in the SAL and <bold>(b)</bold> in the MBL, for
the PCASP, CDP and 2-DS XY. Errors combine systematic and random errors. For
clarity only upper error bounds are shown. The following numbers of SLRs
were performed per flight in the SAL and are shown in panel <bold>(a)</bold>: b920 (2),
b924 (1), b928 (6), b932 (2), b934 (3). One SLR per flight was performed in
the MBL as shown in panel <bold>(b)</bold>.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f05.pdf"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS2">
  <title>Size distributions and shape</title>
      <p id="d1e3978">Figure 5 shows the wing probe size distributions
for each SLR, separated into those measured in the SAL and MBL. The size
distribution in the SAL displays a broad shape which does not change with
increasing or decreasing dust load but simply shifts between higher or
lower volume concentrations. For example, for b924 under large dust loadings
where lidar-derived AODs approached 2.0 (Marenco et al., 2018), the volume concentrations are markedly larger than on other flights
in AER-D (green points in Fig. 5), although the
size distribution shape is much the same. This is in contrast with
measurements over land close to dust sources during Fennec (Ryder et al.,
2013b) where the absence or presence of the coarse and giant modes had a
strong impact on the overall shape of the size distribution, since the
relative proportion of giant particles was observed to increase. The peak of
the volume concentration during AER-D was constantly between 5 and 10 <inline-formula><mml:math id="M193" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
diameter. We observe a fine mode of aerosol at 0.1–0.3 <inline-formula><mml:math id="M194" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, which is
evident when dust concentrations are lower but becomes eclipsed by the
accumulation mode dust during flights with larger dust loadings (e.g. b924).
Section 3.4 shows that the composition of <inline-formula><mml:math id="M195" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 0.5 <inline-formula><mml:math id="M196" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m aerosol in the SAL during AER-D was dominated by
sulfates and salts, thus explaining the different behaviour of this mode.
Liu et al. (2018) examine the composition and behaviour of the
accumulation mode during ICE-D in more detail.</p>
      <p id="d1e4009">In the MBL, a distinct giant mode is evident between 20 and 60 <inline-formula><mml:math id="M197" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
during three flights (b924, b928 and b932: red, green and orange in
Fig. 5b). For flight b928, filter sample analysis
(Sect. 3.4) confirms that this giant mode is
composed of dust rather than sea salt. Higher wind speeds in the MBL, which
may be an indicator of sea salt abundance, are not correlated with the
presence of this giant mode (10–11 ms<inline-formula><mml:math id="M198" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for b924 and b932; 3–5 ms<inline-formula><mml:math id="M199" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for b920, b928 and b934). It is possible that turbulent mixing
from the SAL to the MBL is more likely given a weak inversion and higher
turbulence. Therefore, we also examined whether the strength of the
temperature inversion (calculated using the vertical gradient of potential
temperature) and the strength of turbulence at the inversion (indicated by
the variance of vertical velocity) could be related to the giant particles
present in the MBL. However, we found no obvious connection in these cases.
We note that giant mode particles in the MBL were only present during
flights when there was a significant presence of giant mode particles in the
SAL above: there is a giant mode in Fig. 5b
(flights b924, b928, b932; green, orange, red) only when a higher
concentration of particles in the SAL in the same size range was measured
(Fig. 5a, same colours). When few particles are
measured in the SAL in this size range (b920 and b934, blue and purple), the
MBL giant mode is also absent. Thus, the observations suggest that the giant
MBL mode may be dust being deposited from the overlying SAL towards the
ocean. This has also been suggested by Jaenicke and Schutz (1978) from
aerosol surface observations at Sal, Cape Verde, where giant particles (<inline-formula><mml:math id="M200" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 40 <inline-formula><mml:math id="M201" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m)
were observed to arrive at the site a day after coarse dust particles (6 &lt; <inline-formula><mml:math id="M202" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 60 <inline-formula><mml:math id="M203" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m).</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T5" specific-use="star"><caption><p id="d1e4075">Lognormal mode properties for the number size distribution.
Diameters are given in microns, number concentrations in ambient cm<inline-formula><mml:math id="M204" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. <inline-formula><mml:math id="M205" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">pg</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> represents the median diameter,
<inline-formula><mml:math id="M206" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="normal">g</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> represents the geometric standard deviation and <inline-formula><mml:math id="M207" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">tot</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> represents the total aerosol number concentration.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="7">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">Mode 1</oasis:entry>
         <oasis:entry colname="col5">Mode 2</oasis:entry>
         <oasis:entry colname="col6">Mode 3</oasis:entry>
         <oasis:entry colname="col7">Mode 4</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">SAL</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M208" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mrow><mml:mi>p</mml:mi><mml:mi>g</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">Mean</oasis:entry>
         <oasis:entry colname="col4">0.105</oasis:entry>
         <oasis:entry colname="col5">0.851</oasis:entry>
         <oasis:entry colname="col6">1.580</oasis:entry>
         <oasis:entry colname="col7">32.527</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M209" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="normal">g</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">2.200</oasis:entry>
         <oasis:entry colname="col5">1.181</oasis:entry>
         <oasis:entry colname="col6">1.928</oasis:entry>
         <oasis:entry colname="col7">1.528</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M210" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">tot</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M211" display="inline"><mml:mrow><mml:mn mathvariant="normal">3.91</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M212" display="inline"><mml:mrow><mml:mn mathvariant="normal">8.39</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">0</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M213" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.16</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">1</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M214" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.38</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">4</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M215" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">pg</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">Min</oasis:entry>
         <oasis:entry colname="col4">0.142</oasis:entry>
         <oasis:entry colname="col5">0.838</oasis:entry>
         <oasis:entry colname="col6">2.176</oasis:entry>
         <oasis:entry colname="col7">10.643</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M216" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>g</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">1.658</oasis:entry>
         <oasis:entry colname="col5">1.262</oasis:entry>
         <oasis:entry colname="col6">1.585</oasis:entry>
         <oasis:entry colname="col7">1.300</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">N<inline-formula><mml:math id="M217" display="inline"><mml:msub><mml:mi/><mml:mi mathvariant="normal">tot</mml:mi></mml:msub></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M218" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.14</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M219" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.80</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">0</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M220" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.52</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">0</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M221" display="inline"><mml:mrow><mml:mn mathvariant="normal">4.44</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></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M222" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mrow><mml:mi>p</mml:mi><mml:mi>g</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">Max</oasis:entry>
         <oasis:entry colname="col4">0.089</oasis:entry>
         <oasis:entry colname="col5">0.576</oasis:entry>
         <oasis:entry colname="col6">1.571</oasis:entry>
         <oasis:entry colname="col7">15.421</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M223" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>g</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">2.200</oasis:entry>
         <oasis:entry colname="col5">1.500</oasis:entry>
         <oasis:entry colname="col6">1.957</oasis:entry>
         <oasis:entry colname="col7">1.877</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">N<inline-formula><mml:math id="M224" display="inline"><mml:msub><mml:mi/><mml:mi mathvariant="normal">tot</mml:mi></mml:msub></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M225" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.14</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M226" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.32</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M227" display="inline"><mml:mrow><mml:mn mathvariant="normal">5.47</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">1</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M228" display="inline"><mml:mrow><mml:mn mathvariant="normal">3.75</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></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">MBL</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M229" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mrow><mml:mi>p</mml:mi><mml:mi>g</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">Mean</oasis:entry>
         <oasis:entry colname="col4">0.148</oasis:entry>
         <oasis:entry colname="col5">0.487</oasis:entry>
         <oasis:entry colname="col6">3.675</oasis:entry>
         <oasis:entry colname="col7">7.651</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M230" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>g</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">1.437</oasis:entry>
         <oasis:entry colname="col5">1.900</oasis:entry>
         <oasis:entry colname="col6">1.392</oasis:entry>
         <oasis:entry colname="col7">2.000</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">N<inline-formula><mml:math id="M231" display="inline"><mml:msub><mml:mi/><mml:mi mathvariant="normal">tot</mml:mi></mml:msub></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M232" display="inline"><mml:mrow><mml:mn mathvariant="normal">3.14</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M233" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.42</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">1</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M234" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.38</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">0</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M235" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.08</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">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M236" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mrow><mml:mi>p</mml:mi><mml:mi>g</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">Min</oasis:entry>
         <oasis:entry colname="col4">0.133</oasis:entry>
         <oasis:entry colname="col5">0.686</oasis:entry>
         <oasis:entry colname="col6">3.288</oasis:entry>
         <oasis:entry colname="col7">10.457</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M237" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>g</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">1.483</oasis:entry>
         <oasis:entry colname="col5">1.500</oasis:entry>
         <oasis:entry colname="col6">1.500</oasis:entry>
         <oasis:entry colname="col7">1.300</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">N<inline-formula><mml:math id="M238" display="inline"><mml:msub><mml:mi/><mml:mi mathvariant="normal">tot</mml:mi></mml:msub></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M239" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.35</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M240" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.39</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">0</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M241" display="inline"><mml:mrow><mml:mn mathvariant="normal">6.60</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">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M242" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.27</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></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M243" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mrow><mml:mi>p</mml:mi><mml:mi>g</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">Max</oasis:entry>
         <oasis:entry colname="col4">0.151</oasis:entry>
         <oasis:entry colname="col5">0.458</oasis:entry>
         <oasis:entry colname="col6">3.144</oasis:entry>
         <oasis:entry colname="col7">7.651</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M244" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>g</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4">1.423</oasis:entry>
         <oasis:entry colname="col5">1.872</oasis:entry>
         <oasis:entry colname="col6">1.491</oasis:entry>
         <oasis:entry colname="col7">2.000</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">N<inline-formula><mml:math id="M245" display="inline"><mml:msub><mml:mi/><mml:mi mathvariant="normal">tot</mml:mi></mml:msub></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M246" display="inline"><mml:mrow><mml:mn mathvariant="normal">4.86</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M247" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.81</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">1</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M248" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.88</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mn mathvariant="normal">0</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M249" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.32</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">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d1e5101">Despite careful error analysis and selection of instrumental data, there is
still a large degree of noise as a function of diameter in the wing probe
size distributions shown in Fig. 5, which was
also not indicated in the filter sample PSDs. Therefore, in
Fig. 6, lognormal curves using four lognormal modes
are fitted to the wing probe instrumental data using a least squares
regression (Markwardt, 2008) with mode parameters from
Table 5. The lognormal curves represent a best fit
across the full size range for the instruments available. Differences
between the effective diameter calculated with the best-fit lognormal curves
and the observed PSDs are between 10 % and 15 %, resulting largely from
deviations between the observations and best-fit curve in the CDP size range
(3 to 20 <inline-formula><mml:math id="M250" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6"><caption><p id="d1e5114">AER-D mean logfit size distribution from the MBL (blue) and SAL
(orange). Shading indicates the range between minimum and maximum values, and
the central solid line shows the mean.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f06.pdf"/>

        </fig>

      <p id="d1e5123">It can be seen that the volume concentrations in the SAL are larger than
those in the MBL, as expected due to the higher concentrations of elevated
dust and that the SAL size distribution has a notably different structure.
Dust in the SAL displays a broad size distribution with contributions from
particles over a wide range of sizes (0.3 to 100 <inline-formula><mml:math id="M251" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m), peaking at
5–10 <inline-formula><mml:math id="M252" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. The MBL size distribution has a narrow peak at
<inline-formula><mml:math id="M253" display="inline"><mml:mrow><mml:mi>d</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M254" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and a giant mode contribution at around 20 to
60 <inline-formula><mml:math id="M255" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, where volume concentrations in the MBL mean are actually
larger than the SAL mean. Compared to PSDs over the desert measured with
aircraft during Fennec and SAMUM1 (Ryder et al., 2013b; Weinzierl et al.,
2009), where the volume distributions peak at diameters larger than 10 <inline-formula><mml:math id="M256" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, AER-D has a smaller giant mode contribution, as would be
expected. The AER-D PSD is more in keeping with other aircraft observations
of transported dust, where the volume distributions peak at diameters
between 3 and 10 <inline-formula><mml:math id="M257" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (measured during the following: the Geostationary Earth
Radiation Budget Intercomparison of Longwave and Shortwave radiation (GERBILS) – Johnson and
Osborne, 2011; Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) – Denjean et al., 2016; SAMUM2 – Weinzierl et
al., 2011; the Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) – Weinzierl et al., 2017). Despite some agreement
here, the variation in size across the 3 to 10 <inline-formula><mml:math id="M258" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m size range can
still have a large impact<?pagebreak page17240?> on the dust radiative effect (Tegen and
Lacis, 1996). MBL PSDs under the influence of dust advection were measured
by Kandler et al. (2011b) at Cape Verde. Their observations revealed a
sharp mode at 10 <inline-formula><mml:math id="M259" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, declining steeply at larger sizes, which
contrasts with our modes centred at <inline-formula><mml:math id="M260" display="inline"><mml:mrow><mml:mi>d</mml:mi><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M261" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and 20 to 60 <inline-formula><mml:math id="M262" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. They also found that when air masses had a maritime origin (but
still dominated by dust), the PSD was broadly flat between around 10 and 80 <inline-formula><mml:math id="M263" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, similar to the AER-D MBL PSDs.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><caption><p id="d1e5232">Comparison of wing probe size distributions with size
distributions from filter samples at two magnifications (2000 and 10 000) for
four SLRs. Panels <bold>(a)</bold> and <bold>(b)</bold> show PSDs in the MBL without <bold>(a)</bold> and with <bold>(b)</bold> giant mode
present; <bold>(c)</bold> and <bold>(d)</bold> show PSDs in the SAL. For filter PSDs, solid lines
indicate volume distribution calculated assuming a spherical shape using an
area-equivalent diameter. Dashed lines indicate volume distribution
calculated using a height : maximum axis ratio of <inline-formula><mml:math id="M264" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>:</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula> (see text for more
details).</p></caption>
          <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f07.pdf"/>

        </fig>

      <p id="d1e5272">Size distributions have also been derived from the four filter samples and are
contrasted with the wing probe size distributions in
Fig. 7. Such comparisons have previously been
shown to be challenging due to the different nature of measurement from each
instrument (e.g. Chou et al., 2008; McConnell et al., 2008; Price et al., 2018), and discrepancies are common, particularly with non-spherical
particle geometry. We note that particles measured by the PCASP will be
randomly orientated due to passing into the PCASP nozzle. Larger particles
sampled by the CDP and those measured by<?pagebreak page17241?> the 2-DS and CIP15 may be aligned
horizontally in the atmosphere (e.g. Ulanowski et al., 2007) and measured in this orientation. Also, each technique allocates size using
a different methodology. Additionally, filter sample viewing is likely to
preferentially view the larger cross section of plate-like particles as they
fall flat on the filter substrate.</p>
      <p id="d1e5275">Figure 7 shows that in most cases, the filters size
distribution is greater than that from the wing probes. In the size range
0.5–1 <inline-formula><mml:math id="M265" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m the best agreement is found. In three of the four SLRs, the filter coarse-mode volume distribution exceeds that of the wing probes by an order
of magnitude or more. At <inline-formula><mml:math id="M266" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 0.5 <inline-formula><mml:math id="M267" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m the filter size
distribution shows a much more distinct fine mode than that seen from the
PCASP. Solid lines for the filter samples (blue and orange) in
Fig. 7 indicate volume distribution calculated
assuming a spherical shape using diameter calculated from the area-equivalent
diameter of the fitted ellipse. It is possible that the filter samples
overestimate size, and therefore also volume, if particles are plate-like
and fall flat on the filter substrate. We test whether accounting for this
by including a representation of particle height, using a height : maximum
axis ratio of <inline-formula><mml:math id="M268" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>:</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula> (Chou et al., 2008), can improve the agreement
with the wing probes. This sizing metric is shown by the dashed lines in
Fig. 7. Although accounting for preferential
particle orientation on the filters makes some differences to the derived
size distribution, it is not sufficient to allow agreement with the wing
probe size distributions. It is possible that there were problems with the
filters flow rates measured during AER-D resulting from some combinations of
filter pore sizes and filter supports. SLRs with higher flow rates (b920 R2
and R5) show better agreement with the wing probes
(Fig. 7a and c) and also used filter samples with
the larger pore sizes (0.4 <inline-formula><mml:math id="M269" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m), compared to the other two SLRs
(Fig. 7b and d) which have worse agreement. We
note that for all the SLRs shown, the shape of the coarse-mode size
distribution is the same for both filters and wing probes even if they are
offset. For example, the broad shoulder of the coarse-mode size distribution
can be seen in b928 R2 (Fig. 7b), and the sharper
drop off of the coarse mode can be seen in b920 R5 and b934 R6
(Fig. 7c and d) for both filters and wing probe
size distributions. Additionally, diameters of the peak size distribution
(5–10 <inline-formula><mml:math id="M270" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) are consistent in filters and wing probes for the SAL
(c and d). We also note that the filters PSD is much smoother than that from
the CDP.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T6"><caption><p id="d1e5330">Optical and size properties for the AER-D SAL and MBL campaign
minimum, mean and maximum: optical properties of MEC, SSA, asymmetry parameter (<inline-formula><mml:math id="M271" display="inline"><mml:mi>g</mml:mi></mml:math></inline-formula>) and
extinction coefficient (<inline-formula><mml:math id="M272" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="normal">e</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) are given at 550 nm. Effective
diameter (<inline-formula><mml:math id="M273" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) and VMD are calculated
directly from the 2-DS XY PSD; optical properties are calculated using the
same PSDs and iterated RIs for each SLR.</p></caption><oasis:table frame="topbot"><?xmltex \begin{scaleboxenv}{.94}[.94]?><oasis:tgroup cols="3">
     <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:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">SAL mean (min, max)</oasis:entry>
         <oasis:entry colname="col3">MBL mean (min, max)</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">MEC, m<inline-formula><mml:math id="M274" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> g<inline-formula><mml:math id="M275" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.32 (0.27,0.35)</oasis:entry>
         <oasis:entry colname="col3">0.25 (0.22, 0.29)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">SSA</oasis:entry>
         <oasis:entry colname="col2">0.95 (0.91,0.98)</oasis:entry>
         <oasis:entry colname="col3">0.99 (0.97,0.99)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">g</oasis:entry>
         <oasis:entry colname="col2">0.74 (0.74, 0.74)</oasis:entry>
         <oasis:entry colname="col3">0.73 (0.71, 0.74)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M276" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="normal">e</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, Mm<inline-formula><mml:math id="M277" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">220 (38, 1148)</oasis:entry>
         <oasis:entry colname="col3">77 (27, 139)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M278" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M279" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m</oasis:entry>
         <oasis:entry colname="col2">4.0 (3.6, 4.7)</oasis:entry>
         <oasis:entry colname="col3">4.6 (3.4, 5.5)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">VMD, <inline-formula><mml:math id="M280" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m</oasis:entry>
         <oasis:entry colname="col2">5.5 (5.0, 6.3)</oasis:entry>
         <oasis:entry colname="col3">6.0 (5.7, 6.3)</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup><?xmltex \end{scaleboxenv}?></oasis:table></table-wrap>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8" specific-use="star"><caption><p id="d1e5530">Variation in size with altitude for SLRs: <bold>(a)</bold> effective diameter;
<bold>(b)</bold> maximum diameter measured by the 2-DS XY instrument. Orange circles
represent accumulation mode only; blue diamonds represent the FULL PSD.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f08.pdf"/>

        </fig>

      <p id="d1e5545">The examination the metric of effective diameter is useful, since it takes
into account the contribution of a range of particle sizes.
Figure 8a shows that the effective diameter of the
full size distribution computed from the wing probes is fairly constant with
altitude with no discernible trend, as expected for a well-mixed SAL. A
similar picture is seen for the VMD but with values of around 5 to 6 <inline-formula><mml:math id="M281" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (not shown). No evidence is found for larger particles being more abundant
closer to the base of the SAL, as would be expected due to gravitational
settling. For the SAL the mean (minimum, maximum) <inline-formula><mml:math id="M282" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> value is 4.0 <inline-formula><mml:math id="M283" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (3.6, 4.7) while for the MBL the mean is 4.6 <inline-formula><mml:math id="M284" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (3.4, 5.5).
Variation within the MBL is much greater due to the absence or presence of
the giant mode shown in Fig. 6. Mean (minimum,
maximum) <inline-formula><mml:math id="M285" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> for the accumulation mode is smaller at 1.7 <inline-formula><mml:math id="M286" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
(1.4, 2.0) for the SAL and 1.1 <inline-formula><mml:math id="M287" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (0.7, 1.4) for the MBL, in
agreement with Liu et al. (2018), reflecting the enhanced fine mode in the
MBL size distribution from 0.1 to 0.3 <inline-formula><mml:math id="M288" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameters shown in
Fig. 5. We also note that <inline-formula><mml:math id="M289" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> for flight
b924 in the thick dust layer was 4.3 <inline-formula><mml:math id="M290" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m – not at all different from
other <inline-formula><mml:math id="M291" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> values in typical dust loadings, despite total volume
concentration being much larger. Mean AER-D size parameters of <inline-formula><mml:math id="M292" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and
VMD are given for the SAL and MBL in Table 6.</p>
      <?pagebreak page17243?><p id="d1e5654">In addition to <inline-formula><mml:math id="M293" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, we also show the maximum size (<inline-formula><mml:math id="M294" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) detected
by the 2-DS XY at concentrations greater than 10<inline-formula><mml:math id="M295" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> cm<inline-formula><mml:math id="M296" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (see
Sect. 2.3.2) as a useful indication of transport
of the largest sizes, which can contribute substantially to the mass
fraction and are therefore important to dust biogeochemical cycles.
Figure 8b shows the maximum size detected during AER-D.
The largest value of 80 <inline-formula><mml:math id="M297" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m at 900 m comes from flight b924, during
the intense dust event. Within the SAL, <inline-formula><mml:math id="M298" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> varied between 20 and 80 <inline-formula><mml:math id="M299" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, and the same range was found within the MBL. There is no clear
trend of <inline-formula><mml:math id="M300" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> decreasing with altitude. Particles sized 20 <inline-formula><mml:math id="M301" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
(40 <inline-formula><mml:math id="M302" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) or larger were detected in 100 % (36 %) of the AER-D dust
layers investigated and in 100 % (80 %) of MBL layers. The lack of
decrease in <inline-formula><mml:math id="M303" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">max</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> with altitude during AER-D is similar to that observed
over the desert during SAMUM1 by Weinzierl et al. (2011).</p>
      <p id="d1e5765">The prevalence of coarse particles shown in Fig. 8b is greater than predicted due to settling velocities alone: a 20 <inline-formula><mml:math id="M304" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
particle should fall 5 km in 1.4 days (Li and Osada, 2007), and a
40 <inline-formula><mml:math id="M305" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m particle would take 13 h for the same distance. Therefore,
with the dust age range in AER-D estimated at 17 h to 4.6 days, we would
not expect any 40 <inline-formula><mml:math id="M306" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m particles to be present at all and would only
expect 20 <inline-formula><mml:math id="M307" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m particles at altitudes below 2.4 km, yet 40 <inline-formula><mml:math id="M308" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
sizes were measured over 3 km and 20 <inline-formula><mml:math id="M309" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m sizes were measured at
altitudes over 4 km.</p>
      <p id="d1e5812">The aspect ratio derived from the filter samples, defined as the ratio of the
major to minor fitted-ellipse axes, is shown in
Fig. 9. The results are somewhat noisy in the
larger size ranges due to the relatively small number of particles analysed,
and samples where <inline-formula><mml:math id="M310" display="inline"><mml:mi>n</mml:mi></mml:math></inline-formula> &lt; 10 have been excluded. As expected, larger
particles are more non-spherical in general, with higher median aspect
ratios (between 1.30 and 1.51) for the 5 to 10 <inline-formula><mml:math id="M311" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and 10 to 40 <inline-formula><mml:math id="M312" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m size ranges. This contrasts with the 0.5 to 5 <inline-formula><mml:math id="M313" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m range where
median aspect ratio varied from 1.3 to 1.44 and modal values are 1.3. This
is particularly notable for b928 R2 in the MBL where there were enough giant
mode particles (10–40 <inline-formula><mml:math id="M314" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) counted, showing much larger modal aspect
ratios of 1.5 (median of 1.50). For flight b920 the smallest particles
(0.1–0.5 <inline-formula><mml:math id="M315" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) were more spherical (modal aspect ratios 1.0–1.2, median
values 1.08 and 1.23), though b928 R2 and b934 R6 contrast with this with much
greater fractions of higher aspect ratios for smaller particles (mode aspect
ratios 1.2–1.4, median values of 1.27 and 1.13, a larger tail in the aspect
ratio distribution). This is explained by the composition of these latter two SLRs being more strongly dominated by sea salt with a cuboid shape. Data
representing the accumulation mode and full PSD strongly shadow the smallest
size bin shown, since the data are dominated by smallest particles with the
highest number concentrations. Our median values are slightly lower than the
majority of those reported in the literature. For example, SAMUM1 values were around
1.6 for <inline-formula><mml:math id="M316" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 0.5 <inline-formula><mml:math id="M317" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and 1.3 for smaller particles
(Kandler et al., 2009), while at Praia, Cape Verde, Kandler et al. (2011a) found values of 1.6–1.7 at <inline-formula><mml:math id="M318" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 0.7 <inline-formula><mml:math id="M319" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and values
below 1.4 at <inline-formula><mml:math id="M320" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 0.7 <inline-formula><mml:math id="M321" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, and Chou et al. (2008)
found median values of 1.7 during African Monsoon Multidisciplinary Analysis (AMMA). Contrastingly Rocha-Lima et al. (2018) found lower modal values of 1.3 from ground-based samples during
Fennec.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9" specific-use="star"><caption><p id="d1e5903">Number fraction of particles as a function of aspect ratio from
filter sample analysis for the same four SLRs as shown in
Fig. 7, as a function of size (colours), for the
full PSD (0.1–40 <inline-formula><mml:math id="M322" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, solid black) and accumulation mode PSD (0.1–2.5 <inline-formula><mml:math id="M323" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m). An asterisk indicates numbers were
scaled-up from value shown to allow for
different substrate areas at the higher magnification. The top two panels are samples
from the MBL without <bold>(a)</bold> giant particles and with <bold>(b)</bold> giant particles.
Panels <bold>(c)</bold> and <bold>(d)</bold> are SAL samples. Data are not shown where the number of particles
in a size range is under 10. In each panel, the size range (microns diameter)
and the associated number of particles counted and median aspect ratio are
shown.</p></caption>
          <?xmltex \igopts{width=426.791339pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f09.pdf"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS3">
  <title>Mass loading</title>
      <p id="d1e5945">In order to facilitate comparisons with model data, where typical output is
in terms of dust mass loadings, Fig. 10 shows
dust mass loadings from all the 31 AER-D in situ aircraft profiles,
calculated from the measured size distributions and assuming a typical dust
density of 2.65 g cm<inline-formula><mml:math id="M324" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (Tegen and Fung, 1994) and spherical
particles. The intense dust profiles encountered during certain sections of
flights b923/b924 are highlighted in orange, where dust was elevated further
north around the Canary Islands, and in red where the dust was found at
lower altitudes at around 23<inline-formula><mml:math id="M325" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, since they both show notably higher dust mass
loadings. Due to the presence of a strong coarse and giant mode, mass
loadings are generally high and typically 300–1000 <inline-formula><mml:math id="M326" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M327" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in the
elevated SAL (Fig. 10a, black lines) when AODs
were low to moderate (0.2 to 0.5) (black lines). Exceptionally high values
were found during the intense dust event on 12 August 2015 when values of
mass loading exceeded 1000 <inline-formula><mml:math id="M328" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M329" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and reached a maximum value of
around 4600 <inline-formula><mml:math id="M330" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M331" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. These values are of the order of a factor of
10 larger than those observed in the region previously, which measured up to a
maximum size of 20 <inline-formula><mml:math id="M332" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (Collins et al., 2000; Garrett et al.,
2003).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F10" specific-use="star"><caption><p id="d1e6036">Profiles of aerosol mass loading calculated from in situ size
distributions assuming a dust density of 2.65 g cm<inline-formula><mml:math id="M333" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. <bold>(a)</bold> Total mass
loading for the full size distribution; <bold>(b)</bold> accumulation mode mass loading
(<inline-formula><mml:math id="M334" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 2.5 <inline-formula><mml:math id="M335" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m); <bold>(c)</bold> fraction of mass at sizes greater than 5 <inline-formula><mml:math id="M336" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter;
<bold>(d)</bold> fraction of mass at sizes greater than 20 <inline-formula><mml:math id="M337" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
diameter. Black lines in <bold>(a)</bold> and <bold>(b)</bold> represent all AER-D profiles under
low to medium AODs; red/orange represents the intense dust event with AODs
<inline-formula><mml:math id="M338" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">2.0</mml:mn></mml:mrow></mml:math></inline-formula> (b923/b924) separated by locations where the dust was
elevated (orange) or at lower altitudes (red). In <bold>(c)</bold> and <bold>(d)</bold> grey shading
represents AER-D 10th to 90th percentile range; the black line
represents AER-D mean. Dust mass path values are given in the text.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f10.pdf"/>

        </fig>

      <p id="d1e6121">Figure 10b shows that the mass contained within the
accumulation mode (<inline-formula><mml:math id="M339" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 2.5 <inline-formula><mml:math id="M340" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) is around a factor of 10 lower
than the total mass, indicating that sub-sampling dust properties behind
size-limiting inlets significantly under-samples dust mass. Specifically, we
find that on average 14 % (10th and 90th percentiles at 6 % and
28 %) of total mass is contained within the accumulation mode between
altitudes of 1.5 to 4 km, values in agreement with estimates by Kok et al. (2017). Figure 10c and d further illustrate the
impact of size on the mass loading by showing the fraction of mass contained
at diameters greater than 5 and 20 <inline-formula><mml:math id="M341" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (c and d
respectively). These values are selected since 5 <inline-formula><mml:math id="M342" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m is the diameter
at which models begin to under-represent dust mass concentration compared to
observations (Kok et al., 2017), and few models represent dust particles
larger than 20 <inline-formula><mml:math id="M343" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (Huneeus et al., 2011). On average, around
60 % of the mass is found at sizes greater than 5 <inline-formula><mml:math id="M344" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and 0 %–12 %
at sizes greater than 20 <inline-formula><mml:math id="M345" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m in the SAL between altitudes of 1.5 and 4 km
where most of the mass is found. Within the MBL a greater fraction of mass
is found at large sizes: 70 %–80 % greater than 5 <inline-formula><mml:math id="M346" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and 10 %–20 %
greater than 20 <inline-formula><mml:math id="M347" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. In the extreme, up to 90 % of dust mass can be
found at sizes greater than 5 <inline-formula><mml:math id="M348" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and up to 40 % at sizes greater
than 20 <inline-formula><mml:math id="M349" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m.</p>
      <p id="d1e6202">There appears to be a trend with altitude shown in
Fig. 10c: the mean mass fraction at <inline-formula><mml:math id="M350" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 5 <inline-formula><mml:math id="M351" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m decreases steadily from 0.75 at the surface to 0.23
at 5 km altitude. A decrease is also evident in panel d with the largest
fractions being found towards the bottom of the SAL (excluding the MBL).
These decreases with dust mass as a function of altitude are somewhat in
contrast with the homogeneous distribution of <inline-formula><mml:math id="M352" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> throughout the SAL
shown in Fig. 8. This may be due to the<?pagebreak page17244?> data
shown in Fig. 10 coming from profiles rather than
SLRs, such that more data are available and also that although <inline-formula><mml:math id="M353" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>
represents the full size distribution, as such it is relatively insensitive
to smaller changes in the coarse and giant particle concentration. Either
way, there is clearly evidence of coarser dust particles being more
prevalent towards the bottom of the SAL (and also in the MBL), indicating
deposition processes occurring.</p>
      <p id="d1e6242">Additionally, we have calculated dust mass path (DMP, also known as
integrated column mass loading) values from the mass profiles, where DMP is
the vertically integrated mass of dust per unit area (Evan et al.,
2014). For AER-D low to moderate AODs, mean DMP is 1.0 g m<inline-formula><mml:math id="M354" 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> (minimum
and maximum values of 0.2 and 2.4 g m<inline-formula><mml:math id="M355" 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>). These values are higher than, but within, the bounds of error and variability of those derived from
satellite retrievals in the same geographic region (Evan et al.,
2014). However, DMPs produced by CMIP5 models are much lower (0.05 to 0.46 g m<inline-formula><mml:math id="M356" 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 a multi-model median of 0.26 g m<inline-formula><mml:math id="M357" 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>) – falling at or
below the lower edge of the AER-D values, furthering the argument that
models underestimate dust mass loading due to poor representation of dust
coarse mode. For the intense dust event on 12 August, DMP values are
extremely large, from 3.1 to 6.2 g m<inline-formula><mml:math id="M358" 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 \floatpos{t}?><fig id="Ch1.F11" specific-use="star"><caption><p id="d1e6307">Composition as volume fraction from filter samples in the MBL <bold>(a, b)</bold> and SAL <bold>(c, d)</bold>. B928 R2 <bold>(b)</bold> contained a substantial
giant mode in the MBL (e.g. see Figs. 5 and 7). Individual panels indicate number of
particles sampled; an asterisk indicates numbers were scaled-up from the value shown to
allow for different substrate areas at the higher magnification. The Fe-rich
volume fraction is provided on the right axis with different size ranges
offset. Data are also shown as bulk properties for the full PSD and
accumulation mode (<inline-formula><mml:math id="M359" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 2.5 <inline-formula><mml:math id="M360" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) and size resolved. Data are only
shown when the sample size is greater than 5. Error bars count uncertainties.</p></caption>
          <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f11.pdf"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS4">
  <title>Dust composition</title>
      <p id="d1e6345">Figure 11 shows the size-resolved and bulk (full
PSD and accumulation mode, <inline-formula><mml:math id="M361" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 2.5 <inline-formula><mml:math id="M362" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m only) composition
results for the four filter samples analysed. In general, across all the
samples and all size ranges above diameters of 0.5 <inline-formula><mml:math id="M363" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, the particles
are dominated by alumino-silicates and quartz, with alumino-silicates
forming over 80 % of the composition volume, with quartz typically forming
around 10 % of the volume, though sometimes being up to 20 %, consistent
with Price et al. (2018). Other components are generally low in volume
percentage, with calcium-rich particles providing up to 15 % of volume
content in some samples. Particles<?pagebreak page17245?> dominated by iron are present in low
quantities (and therefore displayed separately on the right-hand axis),
although their contribution is extremely important in controlling shortwave
refractive indices (Sect. 3.5). Fe-rich particles
are present in higher quantities in the SAL cases (0.5 %–2.5 %) compared to
the MBL (0 %–0.9 %). Error bars are noticeably large for Fe-rich particles
due to the relatively low counting statistics. Although there is some
variation in the iron content as a function of particle size, no distinct
pattern is displayed across all the samples, and the uncertainties prevent
definitive conclusions from being drawn. Even when the uncertainties are
reduced by looking at the full PSD vs. accumulation mode only (black circle
and triangle), iron content is higher for the full PSD than the accumulation
mode in the SAL for b920 R5 (1.7 % vs. 1.3 %), whereas for b934 R6 also
in the SAL, iron content is higher in the accumulation mode than for the
full PSD (1.3 % vs. 0.6 %). These values agree well with the range of
hematite content proposed by Balkanski et al. (2007), where values span 0.9 to 2.7 %, though our values will be low-biased as we only include
iron when iron was the dominant component of a particle, and it is evident
that iron is present as a portion of almost all larger particles. Iron is
detected across the full size range in variable amounts; thus, where
absorption is increased due to large particle sizes, it will be further
increased due to elevated iron content.</p>
      <p id="d1e6369">The size range 0.1 to 0.5 <inline-formula><mml:math id="M364" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (shown in dark blue) displays a notably
different composition, in keeping with the different size distribution
displayed for the fine mode (Figs. 5 and 7) indicating a different aerosol type.
Although some fraction of this fine mode is composed of dust particles
(alumino-silicates and quartz), there is always a contribution from sulfate
particles (10 %–40 %). Contributions from sea salt in the MBL fine mode (25 %
and 55 %) are higher than in the SAL, as expected. Samples
B928_R2 and B934_R6 show noticeably higher
thenardite concentrations, possibly indicative of dry saline lake origins
(e.g. Formenti et al., 2003) or sea salt<?pagebreak page17246?> reacted with sulfuric acid. The
high contribution of sea salt in the fine mode in b928 R2
(Fig. 11b) impacts the aspect ratio distributions
for this size range shown in Fig. 9b, where these
small particles are much less spherical and present a rectangular shape in
the SEM imagery, inferred to be a cuboid shape.</p>
      <p id="d1e6379">Figure 11 shows that even within the MBL, the
aerosol content was dominated by dust particles in both cases examined here.
Additionally, during b928 R2 (orange points in
Figs. 5b, and 11b), one of the SLRs when a substantial giant mode was present, the
composition data confirms that this giant mode (purple points) was composed
of dust, being dominated by alumino-silicates, quartz and calcium-rich particles (most likely calcite).</p>
      <p id="d1e6382">Kandler et al. (2009, 2011a) show that the quartz fraction for particles
increases with particle size, particularly for <inline-formula><mml:math id="M365" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 20 <inline-formula><mml:math id="M366" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m.
Our data do not show that quartz content appreciably increases with size,
though this may be due to the relatively large errors on the size-resolved
data, although even the bulk data for the full PSD and accumulation mode PSD
with smaller error bars do not show significant differences in quartz
content. It may also be due to our filter data not extending to such large
size ranges (up to 200 <inline-formula><mml:math id="M367" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) as Kandler et al. (2009).</p>
      <p id="d1e6407">Additionally, in contrast with Liu et al. (2018), we do not detect any
black carbon on the filter samples, which they find present predominantly
between sizes of 0.1 and 0.6 <inline-formula><mml:math id="M368" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. During the analysis of 6500
particles, only one black carbon chain structure was observed. This
difference is unlikely to be due to the pore size of the filter samples (0.2
and 0.4 <inline-formula><mml:math id="M369" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) allowing small black carbon (BC) particles to pass through them, since
our filters collect efficiently over a size range extending below this by
diffusion and impaction (e.g. Lindsley, 2016), and the size
distributions in Fig. 7 clearly show that this
size range is collected. BC loadings for the ICE-D flights shown in Liu et al. (2018) are very low (0.05–1.0 <inline-formula><mml:math id="M370" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M371" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>). The most likely
explanation is that BC particles were not present in sufficient
concentrations to be sampled by the filters.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T7" specific-use="star"><caption><p id="d1e6446">Complex refractive indices at 550 nm derived from filter sample
composition assuming internal mixing. Real part (<inline-formula><mml:math id="M372" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula>) and imaginary part (<inline-formula><mml:math id="M373" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula>).
Values are given for the full size distribution (FULL PSD), accumulation
mode PSD (<inline-formula><mml:math id="M374" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 2.5 <inline-formula><mml:math id="M375" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) and as a function of diameter range
given; n/a indicates that not enough particles were detected to allow RI calculation.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="6">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Size range, <inline-formula><mml:math id="M376" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter</oasis:entry>
         <oasis:entry colname="col2">Sample ID</oasis:entry>
         <oasis:entry colname="col3">B920 R2</oasis:entry>
         <oasis:entry colname="col4">B928 R2</oasis:entry>
         <oasis:entry colname="col5">B920 R5</oasis:entry>
         <oasis:entry colname="col6">B934 R6</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Layer type</oasis:entry>
         <oasis:entry colname="col3">MBL</oasis:entry>
         <oasis:entry colname="col4">MBL</oasis:entry>
         <oasis:entry colname="col5">SAL</oasis:entry>
         <oasis:entry colname="col6">SAL</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">FULL PSD</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M377" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.46</oasis:entry>
         <oasis:entry colname="col4">1.48</oasis:entry>
         <oasis:entry colname="col5">1.48</oasis:entry>
         <oasis:entry colname="col6">1.48</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M378" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.0004</oasis:entry>
         <oasis:entry colname="col4">0.0005</oasis:entry>
         <oasis:entry colname="col5">0.0030</oasis:entry>
         <oasis:entry colname="col6">0.0012</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">ACC PSD</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M379" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.47</oasis:entry>
         <oasis:entry colname="col4">1.49</oasis:entry>
         <oasis:entry colname="col5">1.48</oasis:entry>
         <oasis:entry colname="col6">1.48</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M380" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.0014</oasis:entry>
         <oasis:entry colname="col4">0.0010</oasis:entry>
         <oasis:entry colname="col5">0.0023</oasis:entry>
         <oasis:entry colname="col6">0.0023</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">0.1–0.5</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M381" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.49</oasis:entry>
         <oasis:entry colname="col4">1.54</oasis:entry>
         <oasis:entry colname="col5">1.52</oasis:entry>
         <oasis:entry colname="col6">1.53</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M382" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.0002</oasis:entry>
         <oasis:entry colname="col4">0.0005</oasis:entry>
         <oasis:entry colname="col5">0.0021</oasis:entry>
         <oasis:entry colname="col6">0.0009</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">0.5–1.0</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M383" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.48</oasis:entry>
         <oasis:entry colname="col4">1.50</oasis:entry>
         <oasis:entry colname="col5">1.49</oasis:entry>
         <oasis:entry colname="col6">1.51</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M384" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.0007</oasis:entry>
         <oasis:entry colname="col4">0.0004</oasis:entry>
         <oasis:entry colname="col5">0.0026</oasis:entry>
         <oasis:entry colname="col6">0.0039</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">1–2.5</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M385" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.47</oasis:entry>
         <oasis:entry colname="col4">1.48</oasis:entry>
         <oasis:entry colname="col5">1.48</oasis:entry>
         <oasis:entry colname="col6">1.48</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M386" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.0015</oasis:entry>
         <oasis:entry colname="col4">0.0010</oasis:entry>
         <oasis:entry colname="col5">0.0023</oasis:entry>
         <oasis:entry colname="col6">0.0023</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">2.5–5.0</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M387" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.47</oasis:entry>
         <oasis:entry colname="col4">1.48</oasis:entry>
         <oasis:entry colname="col5">1.49</oasis:entry>
         <oasis:entry colname="col6">1.49</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M388" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.0003</oasis:entry>
         <oasis:entry colname="col4">0.0016</oasis:entry>
         <oasis:entry colname="col5">0.0031</oasis:entry>
         <oasis:entry colname="col6">0.0027</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">5–10</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M389" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.45</oasis:entry>
         <oasis:entry colname="col4">1.48</oasis:entry>
         <oasis:entry colname="col5">1.49</oasis:entry>
         <oasis:entry colname="col6">1.47</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M390" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.0004</oasis:entry>
         <oasis:entry colname="col4">0.0003</oasis:entry>
         <oasis:entry colname="col5">0.0034</oasis:entry>
         <oasis:entry colname="col6">0.0003</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">10–40</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M391" display="inline"><mml:mi>m</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.47</oasis:entry>
         <oasis:entry colname="col4">1.47</oasis:entry>
         <oasis:entry colname="col5">n/a</oasis:entry>
         <oasis:entry colname="col6">n/a</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M392" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.0003</oasis:entry>
         <oasis:entry colname="col4">0.0003</oasis:entry>
         <oasis:entry colname="col5">n/a</oasis:entry>
         <oasis:entry colname="col6">n/a</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

</sec>
<?pagebreak page17247?><sec id="Ch1.S3.SS5">
  <title>Refractive indices</title>
      <p id="d1e6984">Size-resolved and bulk complex refractive indices at 550 nm calculated from
the filter samples' composition are shown in Table 7, and full spectral variability (solar and terrestrial) is shown in the
Supplement, Figs. S2 and S3. Real values in Table 7 representing the FULL PSD and accumulation mode PSD are generally 1.47 to
1.49 and do not vary substantially. These values are relatively low compared
to that expected for dust and may be influenced by the lower real part of
illite in determining the “alumino-silicate mean” refractive index which is
an average of illite and kaolinite. Other refractive indices such as those
of Kandler et al. (2009, 2011a) solely apply kaolinite refractive indices
and produce higher real values. The low values may also be influenced by the
internal volume mixing rule applied here and are consistent with those from
Formenti et al. (2014). Additionally, the percentages of kaolinite and
illite by mass respectively have been shown to vary between <inline-formula><mml:math id="M393" display="inline"><mml:mrow><mml:mn mathvariant="normal">71.1</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">13.5</mml:mn></mml:mrow></mml:math></inline-formula> % and <inline-formula><mml:math id="M394" display="inline"><mml:mrow><mml:mn mathvariant="normal">16.4</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">11.8</mml:mn></mml:mrow></mml:math></inline-formula> % for dust originating from southern
Mali–Algeria to <inline-formula><mml:math id="M395" display="inline"><mml:mrow><mml:mn mathvariant="normal">30.7</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">3.2</mml:mn></mml:mrow></mml:math></inline-formula> % and <inline-formula><mml:math id="M396" display="inline"><mml:mrow><mml:mn mathvariant="normal">54.2</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">6.0</mml:mn></mml:mrow></mml:math></inline-formula> % for dust from
Mali–Mauritania–Western Sahara (Formenti et al., 2014). Real values are
also distinctly higher for the smallest size class, though this has no
impact on the bulk value due to the low volumetric contribution from these
small-sized particles.</p>
      <p id="d1e7035">Much more variability is seen in the imaginary part, largely influenced by
the iron content and its absorbing influence via hematite and goethite. For
the two samples in the SAL, <inline-formula><mml:math id="M397" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula> is the same for both in the accumulation mode
(0.0023) but increases or decreases to 0.0030 or 0.0012 when the coarser
particles are included. To explain this, inspecting the size-resolved data,
it can be seen that for sample b920 R5 <inline-formula><mml:math id="M398" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula> increases with size from 0.0020 to
0.0034 reflecting the increasing iron content with size seen in
Fig. 11c. However, this is not the case for the
second SAL sample (b934 R6) where iron content and <inline-formula><mml:math id="M399" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula> are highest (0.0023 to
0.0039) in the mid-range sizes from 0.5 to 5 <inline-formula><mml:math id="M400" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
(Fig. 11d), while lower <inline-formula><mml:math id="M401" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula> values (0.0003 to
0.0009) are found for <inline-formula><mml:math id="M402" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 0.5 <inline-formula><mml:math id="M403" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and <inline-formula><mml:math id="M404" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 5 <inline-formula><mml:math id="M405" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m due to their lower iron content.</p>
      <p id="d1e7102">Imaginary parts for the MBL are much smaller than those for the SAL
(0.0004–0.0005 compared to 0.0012 to 0.003), reflecting the lower iron
content across all size ranges. Real parts in the MBL are not notably
different to those in the SAL.</p>
      <?pagebreak page17248?><p id="d1e7105">Longwave spectral refractive indices have also been calculated and are shown
in Fig. S3. Here the main controlling factor is the
fraction of sea salt and sulfate-rich particles, which is important for
<inline-formula><mml:math id="M406" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &lt; 0.5 <inline-formula><mml:math id="M407" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and occasionally up to <inline-formula><mml:math id="M408" display="inline"><mml:mrow><mml:mi>d</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M409" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m in the MBL,
and the relative proportion of alumino-silicate and quartz is important for
sizes <inline-formula><mml:math id="M410" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 0.5 <inline-formula><mml:math id="M411" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. The refractive indices of sea salt used
here have zero absorption in the longwave spectrum, so higher salt content
lowers <inline-formula><mml:math id="M412" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula> in the smallest size range. All samples show an increase in
absorption within the atmospheric window between around 8.5 and 10 <inline-formula><mml:math id="M413" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m.
The quartz absorption peak occurs at 9.4 <inline-formula><mml:math id="M414" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m while the
alumino-silicate peak occurs at 9.6 <inline-formula><mml:math id="M415" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Thus, the relative proportions
of these two minerals control the height of each of these peaks, but since
no significant size-resolved change in the quartz : alumino-silicate ratio was
found in Sect. 3.4, any size-resolved changes in
these peaks in the longwave refractive index are negligible.</p>
      <p id="d1e7185">The longwave imaginary parts are substantially higher between 9 and 10 <inline-formula><mml:math id="M416" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, by 2 to 3 times, than those of some of the literature where <inline-formula><mml:math id="M417" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula> is less
than 1.0 (Di Biagio et al., 2017; Fouquart et al., 1987; Volz, 1973; Hess
et al., 1998; Balkanski et al., 2007), although our values are similarly high to
those of both Otto et al. (2009) and Formenti et al. (2014), who used similar internal mixing volume calculations. We purport this to be due
to the assumption of an internally mixed dust aerosol to be inappropriate,
knowing that the dust is actually externally mixed (excepting the complex
nature of iron existing within mixtures), as in Formenti et al. (2014),
though why this assumption produces worse results in the longwave spectrum
is unclear. Other ways of calculating the refractive index based on iron
being internally mixed, while quartz and alumino-silicates are externally
mixed, are possible (e.g. Balkanski et al., 2007), as are other more
complex ways of representing internal and inhomogeneous mixing (Lindqvist
et al., 2014; Nousiainen, 2009), but they are beyond the scope of this work.</p>
</sec>
<sec id="Ch1.S3.SS6">
  <title>Optical properties</title>
      <p id="d1e7208">Figure 12 shows how SSA varied with height for the
accumulation mode and the full size distribution. SSA was fairly constant
with altitude within the SAL. Measured mean (minimum, maximum) accumulation
mode SAL SSAs (black) were 0.97 (0.93, 0.98). MBL values were all greater
than 0.99. Mie-calculated values of SSA for the accumulation mode (orange)
agree with measurements (black) within error bounds, since here agreement in
SSA is tuned by refractive index iterations. Once the full size distribution
had been accounted for, calculated SSA values (green) decrease to 0.95
(0.91, 0.98) for the SAL and to 0.99 (0.97, 0.99) for the MBL. Since larger
particles are more absorbing for a fixed refractive index, this decrease is
expected, and the magnitude of the decrease is dependent on the amount of
coarse particles and also the refractive index. In the MBL, SSA values do
not decrease much since <inline-formula><mml:math id="M418" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> is small (<inline-formula><mml:math id="M419" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.0001</mml:mn><mml:mi>i</mml:mi></mml:mrow></mml:math></inline-formula>); the
addition of a coarse mode of negligible absorption makes little difference
to SSA. However, in the SAL, where derived <inline-formula><mml:math id="M420" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> varies from 0.0005 to
<inline-formula><mml:math id="M421" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.0025</mml:mn><mml:mi>i</mml:mi></mml:mrow></mml:math></inline-formula>, the addition of the full coarse mode causes SSA to drop noticeably.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F12"><caption><p id="d1e7257">Variation in SSA at 550 nm with altitude for SLRs. Black circles
indicate direct measurements taken in-cabin behind inlets and therefore
represent the accumulation mode (ACC PSD) only. Orange circles indicate
calculated properties, representative of the same conditions in-cabin behind
inlets for the ACC PSD. Green diamonds indicate values calculated using the
2-DS-XY FULL PSD covering size ranges 0.1 to 200 <inline-formula><mml:math id="M422" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Green and orange data
points are from Mie calculations;s black represents measurements.</p></caption>
          <?xmltex \igopts{width=213.395669pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f12.pdf"/>

        </fig>

      <p id="d1e7273">Since it is clear from the composition results that aerosol in the SAL is
dominated by dust across all sizes, applying the same <inline-formula><mml:math id="M423" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> for the
accumulation mode to the coarse particles may be appropriate. However, some
variation in dust composition with size is still evident (Sect. 3.4), which is not taken into account in
Fig. 12. The low <inline-formula><mml:math id="M424" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> of <inline-formula><mml:math id="M425" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.0001</mml:mn><mml:mi>i</mml:mi></mml:mrow></mml:math></inline-formula> in the
MBL is representative of highly scattering sea salt or sulfates which
dominate the fine mode in the MBL (Sect. 3.4),
although it is clear that dust particles dominate at larger sizes in the
MBL. Therefore, extending the low value of <inline-formula><mml:math id="M426" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> to the coarse mode in
the MBL is a less reasonable assumption. Therefore, it is likely that the SSA
values in the MBL for the full size distribution shown in
Fig. 12 are overestimates. SSA values calculated
using an RI representative of dust for the coarse mode from filter samples
are discussed later on.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F13" specific-use="star"><caption><p id="d1e7322">Contribution to single scattering albedo from particle size
(<bold>a</bold> SSA vs. <inline-formula><mml:math id="M427" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) and from composition (<bold>b</bold> SSA vs. <inline-formula><mml:math id="M428" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>), separated by
SLRs in the SAL (orange and yellow) and MBL (blue). Small data points
represent the ACC PSD only; large data points represent the FULL PSD.
Asterisks in <bold>(a)</bold> are direct observations behind inlets. Circles represent
calculations using the RI derived from Mie iterations; diamonds represent
calculations using RI derived from composition data from filter samples
assuming internal mixing (four samples). For the FULL PSD with the iterated RI,
the same accumulation mode RI is extended to the coarse mode. For the
filter RI, a size-specific RI is used for the accumulation mode and the FULL PSD (as given in Table 7).</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f13.pdf"/>

        </fig>

      <p id="d1e7362">Theoretically, the variability of the optical properties of dust in the SAL
may be determined by either the dust composition, the dust size
distribution or both. Other elements may also influence the optical
properties, such as particle shape, roughness, hygroscopic growth and
mixing, but they are not considered here as there are few observational
constraints available on these properties from AER-D. In order to determine
the contributions from both particle size (assessed via <inline-formula><mml:math id="M429" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> from the
measured size distribution) and composition (assessed via <inline-formula><mml:math id="M430" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> calculated from two different methods described in Sect. 2.5)
to the variability of SSA, we show both
<inline-formula><mml:math id="M431" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M432" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> as a function of SSA in
Fig. 13, separated into the ACC PSD and FULL PSD
size ranges.</p>
      <p id="d1e7409">It is clear that during AER-D, it was the variability of dust composition
that controlled the variability of SSA rather than the variability of size
distribution. In Fig. 13a for the SAL (orange)
points, it can be seen that the direct observations for<?pagebreak page17249?> the accumulation
mode (orange asterisks, where nephelometer and PSAP scattering and
absorption are used to calculate SSA) are in agreement with Mie simulations
using the ACC PSD (small orange circles). When the coarse-mode size
distribution is then included (large orange circles), effective diameter
increases and there is a slight decrease in SSA. Although <inline-formula><mml:math id="M433" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> does
impact the magnitude of the SSA, within AER-D the shape of the PSD was
relatively stable, with a relatively constant <inline-formula><mml:math id="M434" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>. This meant that the
small variation in size distribution shape had minimal impact in determining
the variability of SSA.</p>
      <p id="d1e7434">Figure 13b shows the variation in SSA as a function
of composition, represented by <inline-formula><mml:math id="M435" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>. Here we show the relationship
between these two variables calculated with different RI datasets: firstly
for RI from the Mie scattering iterations (circles, Sect. 2.5.1) and secondly for RI calculated for filter
sample composition (diamonds, Sect. 2.5.2).
Optical properties are shown for the accumulation mode only (small data
points), and for the FULL PSD (large data points). For dust in the SAL,
Fig. 13b shows a consistent decrease in SSA with
the imaginary part of the refractive index. This relationship becomes more
negative when the full coarse-mode PSD (large symbols) are included because
for a fixed RI, the larger particles exert more absorption. Although there
is some variability between the results from different RI datasets, overall
they show the same trend.</p>
      <p id="d1e7448">Contrastingly to Fig. 13a, Fig. 13b shows that the SSA variability was
strongly influenced by the variability in composition. This is the case for
both accumulation mode observations of SSA and for the full size
distribution. It is not surprising that variability in <inline-formula><mml:math id="M436" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> influences
absorption and therefore SSA. However, the SSA can be influenced by several
factors, including the PSD. Our aim is to investigate which factors
influence the variability of the SSA. Therefore, it is notable that there is
so little variation in the PSD during AER-D that the composition (or
<inline-formula><mml:math id="M437" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>) is the main factor contributing to the variability of the SSA.
This finding is notably the opposite of that found during Fennec, where
the size distribution was the dominant controller of optical properties.
Liu et al. (2018) show that hematite content is important in the
ICE-D/AER-D samples as a controlling factor on optical properties.
Moosmuller et al. (2012) and Caponi et al. (2017) also show
dependencies of refractive index on iron content. This is consistent with
our findings that the calculated refractive index from the filter samples is
strongly influenced by the iron content and its absorbing properties. It
appears that over the Sahara, variations in the PSD (affected by dust age)
have an important impact on SSA, while over the ocean the impacts of
composition (perhaps either by chemical aging or by sampling dust from
different sources) become more important.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F14" specific-use="star"><caption><p id="d1e7476">Comparison of SSAs calculated using different RI methods for
<bold>(a)</bold> the ACC PSD and <bold>(b)</bold> the FULL PSD. Observations are only available for the
accumulation mode, shown in <bold>(a)</bold>. SSA is calculated using RI derived from
filter samples assuming internal and external mixing or iterated RI.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/17225/2018/acp-18-17225-2018-f14.pdf"/>

        </fig>

      <p id="d1e7494">Finally, we compare optical properties calculated with composition data from
the filter samples using both internal and external mixing assumptions
against observations in Fig. 14 for the ACC PSD
(a) and the FULL PSD (b). Observations are available only for the ACC PSD
size range. Figure 14a shows that compared to the
observations of SSA, the external mixing assumption provides closer
agreement with the observations, confirming that the internal mixing
assumption used to derive refractive indices shown in Sect. 3.5 overestimates the absorption, consistent with
previous publications (Formenti et al., 2014).
Figure 14b shows the same<?pagebreak page17250?> results but for the FULL PSD and also those for the iterated RI for the FULL PSD. The internal and
external mixing calculations, when applied to the full size distribution,
allow for the composition of larger particles being dust in the MBL,
contrasting with the iterated RI method which assumes constant composition
across all sizes. For the two MBL SLRs the SSAs drop from 0.99 for the ACC
PSD down to 0.98 and 0.97 for external mixing when the coarse mode and its
composition is accounted for – thus producing SSAs in the MBL similar to
those of the overlying SAL. This is only achieved through analysis of the
coarse-mode aerosol composition within the MBL. SSAs from internal mixing
RIs are also 0.98 and 0.97 for the MBL SLRs, but these are much the same as
those for the accumulation mode. For b934 R6 there is not much variation
between the three methods, while for b 920 R5 the SSA is lower at 0.89 for
internal mixing, compared to 0.96 for the other two methods. This is because
b934 R6 contained more iron in the coarse mode than the other SLRs (see
Fig. 11c) which had a strong impact on lowering
the SSA for an internal mixing assumption. This is not reflected in the
external mixing value due to the non-linearity of the scattering and
absorption properties.</p>
      <p id="d1e7497">Campaign mean optical properties representing the full size distribution in
the SAL and MBL are summarized in Table 6. In
AER-D, MEC in the SAL is higher (0.27–0.35 m<inline-formula><mml:math id="M438" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> g<inline-formula><mml:math id="M439" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula>) compared to
Fennec observations over the Sahara (0.15–0.23 m<inline-formula><mml:math id="M440" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> g<inline-formula><mml:math id="M441" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, Ryder et al., 2013a) as a result of fewer coarse and giant particles. AER-D SAL SSA
values (0.91 to 0.98, mean 0.95) are somewhat higher than those of Fennec
(0.86 to 0.97) for the same RI (Ryder et al., 2013b) and closer to
previously published higher values for transported dust. For example,
(Haywood et al., 2003) values of 0.95–0.98 during the Saharan Dust Experiment (SHADE) and Chen et al. (2011) values of <inline-formula><mml:math id="M442" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.97</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula> during NASA AMMA (NAMMA). AER-D SAL asymmetry
parameters are large at 0.74, unsurprising given the presence of coarse
particles, contributing to forward scattering.</p>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <title>Conclusions</title>
      <p id="d1e7558">Dust in the SAL during the AER-D airborne field campaign from 6 different
flights, 19 in situ SLRs and 31 profiles has been characterized. The flights
were performed in August 2015 between Cape Verde and the Canary Islands. In
particular, a strong focus is given to the presence and contribution from
coarse and giant dust particles through operating wing-mounted
instrumentation intended to sample the full size distribution from 0.1 to
100 <inline-formula><mml:math id="M443" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter. This work fills a research gap by firstly providing in situ
coarse-mode dust observations which cover the full size range and
secondly by providing these observations in the SAL close to the African
continent during the peak dust transport season.</p>
      <p id="d1e7568">Dust sources contributing to the events sampled were located in southern
Algeria, Mali and northern Mauritania, with a well-documented dust hotspot
along the Mali–Algeria border contributing to dust sampled in four out of
five cases. Several events sampled dust which had been uplifted from up to three
separate source regions. Dust age at sampling was determined to be 17 h
to 4.6 days. Dust transport pathways, ages and source locations assessed
with SEVIRI dust RGB satellite imagery were different to paths indicated by
back trajectories, in keeping with Trzeciak et al. (2017) that
back-trajectory models struggle over the convective summertime Sahara.
The vertical structure of the dust was consistent with the conventional model of
the SAL, with elevated dust (<inline-formula><mml:math id="M444" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>–5 km) overlying the MBL,
except in one intense dust event with an AOD of 2.5, with thick dust
concentrated between 500 m and 2.5 km altitude.</p>
      <?pagebreak page17251?><p id="d1e7581">Size distributions spanning 0.1 to 100 <inline-formula><mml:math id="M445" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m were assessed by combining
wing-mounted optical particle counters and shadow probes. The mean <inline-formula><mml:math id="M446" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> for
the SAL (minimum, maximum) was 4.0 <inline-formula><mml:math id="M447" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (3.6, 4.7 <inline-formula><mml:math id="M448" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m), while for
the MBL the mean was 4.6 <inline-formula><mml:math id="M449" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (3.4, 5.5 <inline-formula><mml:math id="M450" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m). The campaign mean
VMD was 5.5 <inline-formula><mml:math id="M451" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. The shape of the measured size distribution did not
vary significantly between dust layers (reflecting <inline-formula><mml:math id="M452" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> values which
were relatively constant both at different altitudes and in different dust
events). Volume size distributions consistently peaked between 5 and 10 <inline-formula><mml:math id="M453" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, even though total volume concentrations were found to increase or
decrease with dust loading. This contrasts with the Fennec results over desert
where the contribution from the coarse mode was highly variable, as was
<inline-formula><mml:math id="M454" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (Ryder et al., 2013b). Within the SAL dust layers, particles with a 20 <inline-formula><mml:math id="M455" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter or larger were detected in 100 % of cases, and
particles 40 <inline-formula><mml:math id="M456" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m or larger were detected in 36 % of cases, at
concentrations over 10<inline-formula><mml:math id="M457" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> cm<inline-formula><mml:math id="M458" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. Based on dust age at sampling time,
more coarse and giant particles were present than expected due to
gravitational sedimentation alone.</p>
      <p id="d1e7706">Giant particles (<inline-formula><mml:math id="M459" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> &gt; 20 <inline-formula><mml:math id="M460" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) were found in the MBL on three out
of five flights. Filter sample analysis for one of these cases confirms that
these giant particles were dust. The shape of the size distribution
indicates similarity to the dust layers above in the SAL and therefore
suggests a high likelihood of dust being deposited from above. Despite this,
the only size metrics which showed evidence of increasing particle size
towards the bottom of the SAL were the mass fraction of particles sized over
5 and 20 <inline-formula><mml:math id="M461" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m.</p>
      <p id="d1e7731">Size distributions from vertical profiles were also used to calculate size-resolved mass loadings. Very large values were found: between 300 and 1000 <inline-formula><mml:math id="M462" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M463" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in the SAL for low to moderate AODs (0.2 to 0.5) and up
to 4600 <inline-formula><mml:math id="M464" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M465" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in an intense dust event. Only 14 % of mass was
found to reside in sizes beneath 2.5 <inline-formula><mml:math id="M466" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, while 60 % resided in
sizes larger than diameters of 5 <inline-formula><mml:math id="M467" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and 0 %–12 % resided at sizes
above 20 <inline-formula><mml:math id="M468" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. The latter two diameters are important, representing respectively sizes where models begin to underestimate the size distribution and where
models typically exclude larger particles (Kok et al., 2017;
Huneeus et al., 2011). Thus, it is clear that a large proportion of mass
resides in the larger size ranges, which will impact biogeochemical cycles
in models if underestimated. DMPs were also calculated for
these profiles giving values between 0.2 and 2.4 g m<inline-formula><mml:math id="M469" 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> (mean of 1.0 g m<inline-formula><mml:math id="M470" 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>), in agreement with satellite-derived
values of Evan et al. (2014) within error bounds.</p>
      <p id="d1e7818">The analysis of four filter samples provided information on size-resolved aspect
ratio, composition, and refractive indices. Modal aspect ratios were 1.2 to
1.4, lower than typically found in the literature. In the SAL,
alumino-silicate particles dominated the composition at sizes above 0.5 <inline-formula><mml:math id="M471" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, followed by quartz, although sulfates and sea salt were present
in significant quantities at sizes beneath 0.5 <inline-formula><mml:math id="M472" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. In the MBL the
situation was similar, with particles sized over 1 <inline-formula><mml:math id="M473" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m being
predominantly dust, though the contribution of sulfates and sea salt
extended up to 1 <inline-formula><mml:math id="M474" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter. The iron-rich fraction was small in the
SAL (0.5 % to 2.5 % by volume fraction) and even smaller in the MBL (0 % to
0.9 %). Although iron content varied with particle size, there was no
consistent behaviour across the small number of samples analysed.</p>
      <p id="d1e7849">Full spectral complex refractive indices were calculated from the filter
samples. At 550 nm, the imaginary part of the refractive index <inline-formula><mml:math id="M475" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> for
the FULL PSD was 0.0012 to 0.0030 in the SAL, strongly influenced by the
volumetric iron content. Real parts were relatively low at 1.48 due to the
low real values contributed by the literature kaolinite data. In general,
refractive indices at 550 nm calculated from two different methods agreed
well. For the full spectrum of data, iterated <inline-formula><mml:math id="M476" display="inline"><mml:mrow><mml:msup><mml:mi>k</mml:mi><mml:mn mathvariant="normal">550</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> values representing
the accumulation mode covered 0.0005 to 0.0025 with a modal value of 0.001.
Refractive indices calculated from composition data and internal mixing
assumptions were found to overestimate absorption, while external mixing
assumptions provided the best agreement with observations.</p>
      <p id="d1e7874">SSAs for the accumulation mode were measured, and SSAs for the full size
distribution were calculated using measured size distributions and derived
refractive indices at 550 nm. Within the SAL, measured SSAs at 550 nm for
the accumulation mode were 0.93–0.98 (mean 0.97), and calculated values for
the full size distribution dropped to 0.91–0.98 (mean 0.95). During AER-D
the SSA still showed a reasonable amount of variability. The contribution of
both PSD and <inline-formula><mml:math id="M477" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula> to the variability of SSA was investigated. Both the shape of
the PSD and <inline-formula><mml:math id="M478" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> varied little, despite total dust concentrations being
variable. Therefore, during AER-D, variability in PSD did not have a strong
effect on SSA. This allowed variations in composition (via the imaginary
part of the refractive index) to control the variability of the SSA. This
contrasts with Fennec where size was strongly the controlling factor. Liu
et al. (2018) show that hematite variability within the accumulation mode
was an important control on SSA during ICE-D. Within the MBL, aerosol in the
accumulation mode was extremely scattering with SSA values above 0.99.
However, once accounting for the coarse-mode particles and coarse-mode-specific composition, SSAs within the MBL were found to be more
absorbing and representative of mineral dust.</p>
      <p id="d1e7895">Over the Atlantic, a significant coarse mode of dust is still present and
contributes to the overall optical properties of dust. Particles larger than
expected from sedimentation processes alone are found. Additionally, the
transport of mass is dominated by the larger particles, which is important
to biogeochemical cycles via deposition of nutrients to the ocean. However,
we find that variability in the optical properties is controlled principally
by the variability in composition. Therefore, in order to appropriately model
the transport of dust and its associated optical properties and mass
impacts, dust models must attempt to capture both the broad size range of
particles detected by measurements and also the variability in composition,
particularly that from absorbing iron oxides.</p>
</sec>

      
      </body>
    <back><notes notes-type="dataavailability">

      <p id="d1e7903">This dataset collection holds datasets from the FAAM BAe-146 aircraft and ground-based measurements
taken in Cape Verde off the coast of Senegal, Africa, during 2015 and 2016 in support of the UK Ice in Clouds Experiment – Dust (UK ICE-D)
project:
<uri>http://catalogue.ceda.ac.uk/uuid/d7e02c75191a4515a28a208c8a069e70</uri> (Bennett, 2015).</p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d1e7909">The supplement related to this article is available online at: <inline-supplementary-material xlink:href="https://doi.org/10.5194/acp-18-17225-2018-supplement" xlink:title="pdf">https://doi.org/10.5194/acp-18-17225-2018-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution">

      <p id="d1e7918">CR designed and carried out the experiments and analysis and wrote the paper.
FM proposed and coordinated the AER-D field campaign. CR, FM, JB and VE designed the flights and aircraft sampling strategy.
CR, RC, JM, HP, DL, PR, JT, TC, MG, HC, KB, JC, GL and BM operated aircraft instruments and processed and/or quality-controlled data.
CR, PF and PA analysed the filter samples. All authors read and commented on the paper.</p>
  </notes><notes notes-type="competinginterests">

      <p id="d1e7924">The authors declare that they have no conflict of interest.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e7930">Airborne data from the BAe 146 were obtained using the BAe 146-301
Atmospheric Research Aircraft operated by Directflight Ltd and managed by
FAAM, which is a joint entity of the NERC and the UK Met Office. ICE-D was
supported by NERC grant number NE/M001954/1 and the Met Office. SAVEX-D
flights were funded by EUFAR TNA (European Union Seventh Framework Programme
grant agreement 312609), and other AER-D flights were funded by the Met
Office. Claire L. Ryder acknowledges NERC support through Independent Research
Fellowship NE/M018288/1. SAVEX-D was supported by projects
PROMETEUII/2014/058 and GV/2014/046 from the Valencia Autonomous Government and CGL2015-70432-R from the Spanish Ministry of Economy and Competitiveness
– European Regional Development Fund. Benjamin J. Murray, James B. McQuaid and Hannah C. Price thank the European
Research Council (ERC) (240449 ICE and 648661 MarineIce) for funding. CEDA
are acknowledged for their efforts in storing and archiving ICE-D FAAM data.
We thank Claudia Di Biagio for providing mineral refractive index data and
useful discussions, Konrad Kandler for providing calcite refractive index
data, Helen Dacre for dust transport discussions, and Graeme Nott for
discussions about wing probe flow distortions.
<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>
Edited by:  Yves Balkanski<?xmltex \hack{\newline}?>
Reviewed by:  Konrad Kandler and three anonymous referees</p></ack><ref-list>
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    <!--<article-title-html>Coarse-mode mineral dust size distributions, composition and optical properties from AER-D aircraft measurements over the tropical eastern Atlantic</article-title-html>
<abstract-html><p>Mineral dust is an important component of the climate system, affecting the
radiation balance, cloud properties, biogeochemical cycles, regional
circulation and precipitation, as well as having negative effects on
aviation, solar energy generation and human health. Dust size and composition
has an impact on all these processes. However, changes in dust size
distribution and composition during transport, particularly for coarse
particles, are poorly understood and poorly represented in climate models.
Here we present new in situ airborne observations of dust in the Saharan Air
Layer (SAL) and the marine boundary layer (MBL) at the beginning of its
transatlantic transport pathway, from the AERosol
Properties – Dust (AER-D) fieldwork in August 2015,
within the peak season of North African dust export. This study focuses on
coarse-mode dust properties, including size distribution, mass loading,
shape, composition, refractive indices and optical properties. Size
distributions from 0.1 to 100&thinsp;µm diameter (<i>d</i>) are presented, fully
incorporating the coarse and giant modes of dust. Within the MBL, mean
effective diameter (<i>d</i><sub>eff</sub>) and volume median diameter (VMD) were 4.6 and 6.0&thinsp;µm respectively, giant particles with a mode at
20–30&thinsp;µm were observed, and composition was dominated by quartz and
alumino-silicates at <i>d</i>&thinsp;&gt;&thinsp;1&thinsp;µm. Within the SAL, particles
larger than 20&thinsp;µm diameter were always present up to 5&thinsp;km altitude, in
concentrations over 10<sup>−5</sup>&thinsp;cm<sup>−3</sup>, constituting up to 40&thinsp;% of
total dust mass. Mean <i>d</i><sub>eff</sub> and VMD were 4.0 and 5.5&thinsp;µm
respectively. Larger particles were detected in the SAL than can be explained
by sedimentation theory alone. Coarse-mode composition was dominated by
quartz and alumino-silicates; the accumulation mode showed a strong
contribution from sulfate-rich and sea salt particles. In the SAL, measured
single scattering albedos (SSAs) at 550&thinsp;nm representing <i>d</i>&thinsp;&lt;&thinsp;2.5&thinsp;µm were
0.93 to 0.98 (mean 0.97). Optical properties calculated for the full
size distribution (0.1&thinsp;&lt;&thinsp;<i>d</i>&thinsp;&lt;&thinsp;100&thinsp;µm) resulted in lower
SSAs of 0.91–0.98 (mean 0.95) and mass extinction coefficients of 0.27–0.35&thinsp;m<sup>2</sup>&thinsp;g<sup>−1</sup> (mean 0.32&thinsp;m<sup>2</sup>&thinsp;g<sup>−1</sup>). Variability in SSA was mainly
controlled by variability in dust composition (principally iron) rather than
by variations in the size distribution, in contrast with previous observations
over the Sahara where size is the dominant influence. It is important that
models are able to capture the variability and evolution of both dust
composition and size distribution with transport in order to accurately
represent the impacts of dust on climate. These results provide a new SAL
dust dataset, fully representing coarse and giant particles, to aid model
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