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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-17-7891-2017</article-id><title-group><article-title>Optical, physical and chemical properties of aerosols transported to a coastal site in the western Mediterranean: a focus on primary marine aerosols</article-title>
      </title-group><?xmltex \runningtitle{Optical, physical and chemical properties of aerosols transported}?><?xmltex \runningauthor{M. Claeys et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Claeys</surname><given-names>Marine</given-names></name>
          <email>marine.claeys@umr-cnrm.fr</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Roberts</surname><given-names>Greg</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Mallet</surname><given-names>Marc</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Arndt</surname><given-names>Jovanna</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-8103-6106</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Sellegri</surname><given-names>Karine</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5 aff6">
          <name><surname>Sciare</surname><given-names>Jean</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Wenger</surname><given-names>John</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-4109-976X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Sauvage</surname><given-names>Bastien</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-3410-2139</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>CNRM, Centre National de Recherches Météorologiques UMR3589, Météo-France/CNRS, Toulouse, France</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Scripps Institution of Oceanography, Center for Atmospheric Sciences and Physical Oceanography, La Jolla, USA</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Department of Chemistry and Environmental Research Institute, University College Cork, Cork, Ireland</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>LaMP, Laboratoire de Météorologie Physique CNRS UMR6016, Observatoire de Physique du Globe de Clermont-Ferrand, Université Blaise Pascal,
Aubière, France</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>LSCE, Laboratoire des Sciences du Climat et de l'Environnement, Unité Mixte CEA-CNRS-UVSQ, CEA/Orme des Merisiers, 91191 Gif-sur-Yvette, France</institution>
        </aff>
        <aff id="aff6"><label>6</label><institution>Energy Environement Water Research Center, The Cyprus Institute, 2121 Nicosia, Cyprus</institution>
        </aff>
        <aff id="aff7"><label>7</label><institution>LA, Laboratoire d'Aérologie, Observatoire Midi-Pyrénées, CNRS/IRD/Université de Toulouse, 14, Avenue Édouard Belin, 31400 Toulouse, France</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Marine Claeys (marine.claeys@umr-cnrm.fr)</corresp></author-notes><pub-date><day>30</day><month>June</month><year>2017</year></pub-date>
      
      <volume>17</volume>
      <issue>12</issue>
      <fpage>7891</fpage><lpage>7915</lpage>
      <history>
        <date date-type="received"><day>8</day><month>July</month><year>2016</year></date>
           <date date-type="rev-request"><day>3</day><month>August</month><year>2016</year></date>
           <date date-type="rev-recd"><day>12</day><month>April</month><year>2017</year></date>
           <date date-type="accepted"><day>27</day><month>April</month><year>2017</year></date>
      </history>
      <permissions>
<license license-type="open-access">
<license-p>This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/3.0/">https://creativecommons.org/licenses/by/3.0/</ext-link></license-p>
</license>
</permissions><self-uri xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017.html">This article is available from https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017.html</self-uri>
<self-uri xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017.pdf</self-uri>


      <abstract>
    <p>As part of the ChArMEx-ADRIMED campaign (summer 2013), ground-based
in situ observations were conducted at the Ersa site (northern tip of
Corsica; 533 m a.s.l.) to characterise the optical, physical and chemical
properties of aerosols. During the observation period, a major influence of
primary marine aerosols was detected (22–26 June), with a mass concentration
reaching up to 6.5 <inline-formula><mml:math id="M1" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M2" 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 representing more than 40 % of the
total PM<inline-formula><mml:math id="M3" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass concentration. Its relatively low ratio of chloride to
sodium (average of 0.57) indicates a fairly aged sea salt aerosol at
Ersa. In this work, an original data set, obtained from online real-time
instruments (ATOFMS, PILS-IC) has been used to characterise the ageing of
primary marine aerosols (PMAs). During this PMA period, the mixing of fresh and aged PMAs was found
to originate from both local and regional (Gulf of Lion) emissions, according
to local wind measurements and FLEXPART back trajectories. Two different
aerosol regimes have been identified: a dust outbreak (dust) originating from
Algeria/Tunisia, and a pollution period with aerosols originating from
eastern
Europe, which includes anthropogenic and biomass burning sources (BBP). The
optical, physical and chemical properties of the observed aerosols, as well as
their local shortwave (SW) direct radiative effect (DRE) in clear-sky
conditions, are compared for these three periods in order to assess the
importance of the direct radiative impact of PMAs compared to other sources
above the western Mediterranean Basin.</p>
    <p>As expected, AERONET retrievals indicate a relatively low local SW DRF during
the PMA period with mean values of <inline-formula><mml:math id="M4" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>11 <inline-formula><mml:math id="M5" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4 at the surface and
<inline-formula><mml:math id="M6" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>8 <inline-formula><mml:math id="M7" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3 W m<inline-formula><mml:math id="M8" 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> at the top of the atmosphere (TOA). In comparison, our
results indicate that the dust outbreak observed at our site during the
campaign, although of moderate intensity (AOD of 0.3–0.4 at 440 nm and
column-integrated SSA of 0.90–0.95), induced a local instantaneous SW DRF
that is nearly 3 times the effect calculated during the PMA period, with maximum
values up to <inline-formula><mml:math id="M9" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>40 W m<inline-formula><mml:math id="M10" 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> at the surface. A similar range of values were
found for the BBP period to those during the dust period (SW DRF at the surface
and TOA of <inline-formula><mml:math id="M11" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>23 <inline-formula><mml:math id="M12" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 6 and <inline-formula><mml:math id="M13" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>15 <inline-formula><mml:math id="M14" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4 W m<inline-formula><mml:math id="M15" 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> respectively).</p>
    <p>The multiple sources of measurements at Ersa allowed the detection of a PMA-dominant period and their characterisation in terms of ageing, origin,
transport, optical and physical properties and direct climatic impact.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p>The Mediterranean Basin is a crossroad for air masses bringing
different types of aerosols, both from natural and anthropogenic origins
<xref ref-type="bibr" rid="bib1.bibx48" id="paren.1"/>. Of these aerosols, primary marine aerosols
(PMAs; mainly composed of sea salt and to a lesser extent of organic matter)
are important because they are always present over the Mediterranean Basin
and compose the main part of background aerosols over the Mediterranean
<xref ref-type="bibr" rid="bib1.bibx67" id="paren.2"/>. They are able to chemically react with other aerosol
species, act as cloud condensation nuclei (CCN) and also interact with solar
and thermal radiations due to their large size range
<xref ref-type="bibr" rid="bib1.bibx44 bib1.bibx43 bib1.bibx45 bib1.bibx50 bib1.bibx80" id="paren.3"/>. At the global scale, <xref ref-type="bibr" rid="bib1.bibx6" id="text.4"/> estimated
that the contribution of marine aerosols was equivalent to half of the total
direct radiative forcing (DRF), while <xref ref-type="bibr" rid="bib1.bibx92" id="text.5"/> found a
contribution of one-third of the total DRF. However, their contribution is
highly variable in time and space due to spatial variations in wind speed
and long-range transport of marine aerosols. At the regional scale and over
the Mediterranean Basin, <xref ref-type="bibr" rid="bib1.bibx75" id="text.6"/> indicate that the contribution
of sea salt particles to the total aerosol loading and optical depth ranges
from 1 to 10<inline-formula><mml:math id="M16" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="italic">%</mml:mi></mml:mrow></mml:math></inline-formula>. They report aerosol optical depth (AOD) around 0.15–0.20
(at 865 nm) within the sea salt aerosol plume during strong-wind (e.g.
Mistral and Tramontane) events. In addition, <xref ref-type="bibr" rid="bib1.bibx59" id="text.7"/> reported a
high correlation between AOD (at 500 nm) and wind speed, with AOD values of
0.3–0.4 at moderately high wind speed – most likely related to the increase
in PMA. Consequently, the persistent and punctually elevated AOD due to PMAs can have a significant impact on the radiative budget of the
Mediterranean Basin. This high variability in terms of PMA loading and
optical, physical and chemical properties leads to significant uncertainties in
the quantification of regional radiative impact, both for direct and indirect
effects <xref ref-type="bibr" rid="bib1.bibx28 bib1.bibx85" id="paren.8"/>. Finally, it should
be noted that most past studies have documented aerosol properties in the
eastern part of the Mediterranean Basin (Crete <xref ref-type="bibr" rid="bib1.bibx56 bib1.bibx5 bib1.bibx78 bib1.bibx47" id="altparen.9"/>; Greece <xref ref-type="bibr" rid="bib1.bibx11" id="altparen.10"/>), even
though many studies also took place in the central <xref ref-type="bibr" rid="bib1.bibx55 bib1.bibx20" id="paren.11"/> and western <xref ref-type="bibr" rid="bib1.bibx81 bib1.bibx15 bib1.bibx68 bib1.bibx37" id="paren.12"/> Mediterranean Basin.</p>
      <p>In that context, the aim of this study is to characterise the optical,
physical and chemical properties of PMAs compared to the other major aerosol
sources affecting the western Mediterranean Basin.</p>
      <p>This work has taken place in the frame of the ChArMEx-ADRIMED (Chemistry-Aerosols Mediterranean Experiment – Aerosol Direct Radiative Impact on the
regional climate in the MEDiterranean region) project
(<uri>https://charmex.lsce.ipsl.fr</uri>) which took place in the western
Mediterranean Basin during summer 2013 <xref ref-type="bibr" rid="bib1.bibx53" id="paren.13"/>, and we used
the real-time measurements taken at the remote ground-based Ersa
atmospheric station situated at Cap Corse (42.9694<inline-formula><mml:math id="M17" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N,
9.3803<inline-formula><mml:math id="M18" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W, altitude of 533 m a.s.l.).</p>
      <p>The first section of this paper (Sect. 2) describes the instrumentation
deployed at the Ersa station and the FLEXible PARTicle (FLEXPART) model configuration used to
identify air mass origins at the station. Periods of the field campaign
affected by the major aerosol sources are then discussed (Sect. 3.1 and 3.3)
using chemical and physical measurements, as well as back-trajectory analysis
and direct radiative effects. Finally, meteorological observations recorded
near the sample site (Ersa) during a period characterised by a particularly
strong source of PMA is used to address the dependence of PMA mass
concentration and ageing to local and regional wind speed (Sect. 3.2.2).</p>
</sec>
<sec id="Ch1.S2">
  <title>Method</title>
<sec id="Ch1.S2.SS1">
  <title>Atmospheric station and instrumental set-up</title>
      <p>The research atmospheric station of Ersa is located at the northernmost part
of Corsica (Cap Corse; 42.9694<inline-formula><mml:math id="M19" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 9.3803<inline-formula><mml:math id="M20" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W). Its altitude is 533 m above sea level (a.s.l.), and it is surrounded by the
Mediterranean sea on its northern, eastern and western sides and by mountains
(<inline-formula><mml:math id="M21" display="inline"><mml:mo>≃</mml:mo></mml:math></inline-formula> 1000 m a.s.l.) on its southern side. The station is located in a
remote area, with minimal influence of local anthropogenic emissions. A more
detailed description of the station is given by <xref ref-type="bibr" rid="bib1.bibx53" id="text.14"/>.</p>
      <p>This station is equipped to provide in situ measurement of the aerosol
physical properties, including number concentration and number size
distribution, using a Scanning Mobility Particle Sizer (SMPS 3081, TSI INC.),
an Optical Particle Sizer (OPS 3330, TSI INC.) and an Aerodynamic Particle
Sizer (APS 3321, TSI INC.) to characterise both submicron and supermicron
aerosol particles. Aerosol size distributions was achieved using two sampling
inlets. The first one was a PM<inline-formula><mml:math id="M22" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> head inlet, in which the airflow was
dried using a Nafion dryer (TSI INC.) to a relative humidity below 40 % and
then divided into several paths to the OPS, SMPS and a condensation particle
counter (CPC 3010, TSI INC.). The second head inlet was a PM<inline-formula><mml:math id="M23" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">20</mml:mn></mml:msub></mml:math></inline-formula> with a
flow rate of 1 L min<inline-formula><mml:math id="M24" 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> that sampled for the APS. The flow rate reaching
the other instruments was 1 L min<inline-formula><mml:math id="M25" 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 the OPS and 0.5  L min<inline-formula><mml:math id="M26" 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
the SMPS. The CPC measured the total number aerosol concentration for
electric mobility diameters larger than 10 nm. The SMPS counted the number of
particles per size bins from 10 to 500 nm, while the APS measured the number of particles per size bins from 0.5 to 20 <inline-formula><mml:math id="M27" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and the OPS
from 0.3 to 10 <inline-formula><mml:math id="M28" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m at ambient RH.</p>
      <p>Optical corrections to the OPS size distributions are negligible when
accounting for the refractive indices associated with the different particle
types. We considered the particles as spherical (shape factor equal to 1).</p>
      <p>Particulate matter below 1 and 10 <inline-formula><mml:math id="M29" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (PM<inline-formula><mml:math id="M30" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math id="M31" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula>) were measured at the station on an hourly
basis using a TEOM-FDMS (Thermo Environment, model 1405-F) and a TEOM (Thermo Environment, model1400) respectively.</p>
      <p>Aerosol optical instruments were also deployed (nephelometer TSI INC. at three wavelengths, MAAP) to determine light
scattering and absorption properties of aerosols. The nephelometer measured the scattered and backscattered
coefficients at three wavelengths, 450 (blue), 550 (green) and 700 nm (red) with a PM<inline-formula><mml:math id="M32" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> head inlet
(flow rate of 40 L min<inline-formula><mml:math id="M33" 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>), while the MAAP instrument (Multi Angle Absorption Photometer, Thermo Scientific)
measured the concentration of PM<inline-formula><mml:math id="M34" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> black carbon from the absorption of particles at the 670 nm wavelength.
The nephelometer provides the scattering coefficient (not directly linked to the concentration of particles),
associated with an indication of the size of aerosols through the spectral dependence of the scattering
coefficient between two wavelengths. The nephelometer data are corrected for truncation according to
the <xref ref-type="bibr" rid="bib1.bibx1" id="text.15"/> method for the total aerosol population. Correction factors of
1.29, 1.29 and 1.26 are applied to the scattering coefficients at the wavelengths 450, 550 and 700 nm respectively.</p>
      <p>The PILS-IC measurements were taken using a Particle Into Liquid Sampler
(PILS, <xref ref-type="bibr" rid="bib1.bibx65" id="altparen.16"/>) running at 16.8 (<inline-formula><mml:math id="M35" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.5) LPM and
coupled with two ion chromatographs (IC) for the determination of the major
cations and anions. More details on this instrumentation and its
comparability with other real-time aerosol analysers can be found in
<xref ref-type="bibr" rid="bib1.bibx93 bib1.bibx79 bib1.bibx41 bib1.bibx14 bib1.bibx8" id="text.17"/>. Basic and acidic annular denuders
(3-channel, URG Corp., USA) were mounted upstream of the PILS instrument and
downstream of a PM10 inlet having a 50<inline-formula><mml:math id="M36" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="italic">%</mml:mi></mml:mrow></mml:math></inline-formula> cut-off diameter of 10 <inline-formula><mml:math id="M37" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m at
16.67 LPM. Ambient concentrations of ions were corrected from blanks
performed every day for 1 h and achieved by placing a total filter upstream of
the sampling system. Liquid flow rates of the PILS were delivered by
peristaltic pumps and set to 1.5 mL min<inline-formula><mml:math id="M38" 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 producing steam inside the PILS
and 0.37 (<inline-formula><mml:math id="M39" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.02)  mL min<inline-formula><mml:math id="M40" 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 rinsing the impactor. Cation measurements
were taken using an IC (Dionex, model ICS1100) equipped with a 2 mm-diameter
AutoSuppression, Cation Self-Regenerating Suppressor (CSRS), a 2 mm-diameter CS-12 pre-column and column, and a 100 <inline-formula><mml:math id="M41" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>L injection loop.
Analyses were performed in isocratic mode at 20 mM of methanesulfonic acid
(MSA) at a flow rate of 0.25 mL min<inline-formula><mml:math id="M42" 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 the quantitative determination of the
five major cations (Na<inline-formula><mml:math id="M43" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>, NH<inline-formula><mml:math id="M44" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>, K<inline-formula><mml:math id="M45" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>, Mg<inline-formula><mml:math id="M46" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula>, Ca<inline-formula><mml:math id="M47" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula>) every
12 min. Based on these IC settings, the detection limit (2<inline-formula><mml:math id="M48" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>) for
cations was typically 0.1 ppb, which corresponds to an atmospheric
concentration of <inline-formula><mml:math id="M49" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 ng m<inline-formula><mml:math id="M50" 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>. Calibration was performed every 2 weeks
for concentrations ranging from 10 to 800 ppb and showed a drift below 5<inline-formula><mml:math id="M51" display="inline"><mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="italic">%</mml:mi></mml:mrow></mml:math></inline-formula>
for each cation between the beginning and the end of the campaign. Anion
measurements were taken using an IC (Dionex, model ICS2000) equipped with
a 2 mm-diameter Auto-Suppression, Anion Self-Regenerating Suppressor (ASRS),
a 2 mm-diameter AS-11 HC pre-column and column, and a 500 <inline-formula><mml:math id="M52" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>L injection
loop. Analyses were performed in isocratic mode at 10 mM of KOH at a flow rate
of 0.25 mL min<inline-formula><mml:math id="M53" 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 the quantitative determination of the 5 anions
(methanesulfonate, Cl<inline-formula><mml:math id="M54" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula>, NO<inline-formula><mml:math id="M55" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>, SO<inline-formula><mml:math id="M56" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math></inline-formula>, oxalate) every 24 min. Based on these IC settings, the detection limit (2<inline-formula><mml:math id="M57" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>) for anions
was typically 0.1 ppb, which corresponds to an atmospheric concentration of
<inline-formula><mml:math id="M58" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 1 ng m<inline-formula><mml:math id="M59" 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>. Calibration was performed every 2 weeks for concentrations
ranging from 10 to 800 ppb and showed a drift below 5<inline-formula><mml:math id="M60" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="italic">%</mml:mi></mml:mrow></mml:math></inline-formula> for each anion
between the beginning and the end of the campaign.
To our best knowledge, this is the first time that PILS-IC measurements are reported in PM<inline-formula><mml:math id="M61" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula>, providing a unique
opportunity to document water-soluble supermicron ions and sea salt in particular. Quality control of the PILC-IC data was
successfully performed by comparison with PM<inline-formula><mml:math id="M62" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> filter (Teflon)-based ion measurements taken in parallel on a 12 h time
basis (Leckel, SEQ47/50 model running at 2.3 m<inline-formula><mml:math id="M63" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:math></inline-formula> h<inline-formula><mml:math id="M64" 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>), with discrepancies typically less than 20<inline-formula><mml:math id="M65" display="inline"><mml:mrow><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="italic">%</mml:mi></mml:mrow></mml:math></inline-formula> for the major anions/cations.</p>
      <p>PMA concentration was calculated using these data and the following formula
<xref ref-type="bibr" rid="bib1.bibx9" id="paren.18"/>:

                <disp-formula specific-use="align"><mml:math id="M66" display="block"><mml:mtable displaystyle="true"><mml:mtr><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mo>[</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">PMA</mml:mi></mml:mrow><mml:mo>]</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mo>=</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>[</mml:mo><mml:msup><mml:mrow class="chem"><mml:mi mathvariant="normal">Cl</mml:mi></mml:mrow><mml:mo>-</mml:mo></mml:msup><mml:mo>]</mml:mo><mml:mo>+</mml:mo><mml:mo>[</mml:mo><mml:msup><mml:mrow class="chem"><mml:mi mathvariant="normal">Na</mml:mi></mml:mrow><mml:mo>+</mml:mo></mml:msup><mml:mo>]</mml:mo><mml:mo>+</mml:mo><mml:mo>[</mml:mo><mml:msup><mml:mrow class="chem"><mml:mi mathvariant="normal">ss</mml:mi><mml:mo>-</mml:mo><mml:mi mathvariant="normal">Mg</mml:mi></mml:mrow><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup><mml:mo>]</mml:mo><mml:mo>+</mml:mo><mml:mo>[</mml:mo><mml:msubsup><mml:mrow class="chem"><mml:mi mathvariant="normal">ss</mml:mi><mml:mo>-</mml:mo><mml:mi mathvariant="normal">SO</mml:mi></mml:mrow><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup><mml:mo>]</mml:mo></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mo>+</mml:mo><mml:mo>[</mml:mo><mml:msup><mml:mrow class="chem"><mml:mi mathvariant="normal">ss</mml:mi><mml:mo>-</mml:mo><mml:mi mathvariant="normal">Ca</mml:mi></mml:mrow><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup><mml:mo>]</mml:mo><mml:mo>+</mml:mo><mml:mo>[</mml:mo><mml:msup><mml:mrow class="chem"><mml:mi mathvariant="normal">ss</mml:mi><mml:mo>-</mml:mo><mml:mi mathvariant="normal">K</mml:mi></mml:mrow><mml:mo>+</mml:mo></mml:msup><mml:mo>]</mml:mo><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula>

            where [ss-X]<inline-formula><mml:math id="M67" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula>[Na<inline-formula><mml:math id="M68" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>] <inline-formula><mml:math id="M69" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 0.13, 0.251, 0.039
and 0.036 corresponding to Mg<inline-formula><mml:math id="M70" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula>, SO<inline-formula><mml:math id="M71" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math></inline-formula>, Ca<inline-formula><mml:math id="M72" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula> and K<inline-formula><mml:math id="M73" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>
respectively. The ACSM measured the chemical composition of non-refractory
PM<inline-formula><mml:math id="M74" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula>, including organic matter (OM), nitrate (NO<inline-formula><mml:math id="M75" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>), sulfate (SO<inline-formula><mml:math id="M76" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:math></inline-formula>),
ammonium (NH<inline-formula><mml:math id="M77" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:math></inline-formula>), chloride (Cl), with a time resolution of 30 min.
The chemical composition of non-refractory submicron aerosol has been continuously monitored using a Quadrupole Aerosol Chemical
Speciation Monitor (Aerodyne Research Inc.), which has been described in detail by <xref ref-type="bibr" rid="bib1.bibx61" id="text.19"/>. Briefly, PM<inline-formula><mml:math id="M78" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula>
aerosols are sampled at 3 L min<inline-formula><mml:math id="M79" 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> (from a PM<inline-formula><mml:math id="M80" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> cyclone inlet) and then subsampled at 85 mL min<inline-formula><mml:math id="M81" 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>
(volumetric flow) through an aerodynamic lens, focusing submicron particles (40–1000 nm aerodynamic diameter, AD) onto
a 600 C-heated conical tungsten vaporiser where non-refractory material is flash vaporised and quasi-instantaneously ionised
by electron impact at 70 eV. Briefly, the instrument calibration has been performed following the recommendation of
<xref ref-type="bibr" rid="bib1.bibx42" id="text.20"/> and <xref ref-type="bibr" rid="bib1.bibx61" id="text.21"/>, where generated monodisperse 300 nm A.D. ammonium nitrate
particles are injected into both ACSM and a CPC at different concentrations. It has
been successfully compared with 15 other aerosol mass spectrometers <xref ref-type="bibr" rid="bib1.bibx13 bib1.bibx30" id="paren.22"/>.
Quality control of ACSM data was successfully performed by comparison of PM<inline-formula><mml:math id="M82" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> (sum of chemical species measured by
ACSM and MAAP; considering that BC aerosols are mainly PM<inline-formula><mml:math id="M83" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula>) with PM<inline-formula><mml:math id="M84" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> obtained with SMPS (with density of 1.5).</p>
      <p>The ATOFMS (aerosol time-of-flight mass spectrometer), deployed by University College Cork, measured the vacuum aerodynamic
diameter of the individual particles and their chemical composition. A detailed description of the ATOFMS (TSI INC. model 3800)
can be found elsewhere <xref ref-type="bibr" rid="bib1.bibx34" id="paren.23"/>. Briefly, it consists of an aerodynamic focusing lens (TSI
AFL100;
<xref ref-type="bibr" rid="bib1.bibx89" id="altparen.24"/>) that transmits particles in the diameter range 100–3000 nm, a particle sizing region, and a bipolar
reflection time-of-flight mass spectrometer. Single particles are desorbed/ionised using a pulsed Nd<inline-formula><mml:math id="M85" display="inline"><mml:mo>:</mml:mo></mml:math></inline-formula>YAG laser
(<inline-formula><mml:math id="M86" display="inline"><mml:mi mathvariant="italic">λ</mml:mi></mml:math></inline-formula> = 266 nm, <inline-formula><mml:math id="M87" display="inline"><mml:mo>≃</mml:mo></mml:math></inline-formula> 1 mJ pulse<inline-formula><mml:math id="M88" 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>). Positive and negative ion mass spectra of individual aerosol particles are obtained
which enable identification of the chemical constituents. The AFL reduces the transmission efficiency of supermicron particles, while
variability in the desorption/ionisation laser influence results in qualitative mass spectral signals.</p>
      <p>The aerosol optical properties were retrieved from the AERONET/PHOTONS
network. We used here the level 1.5 data obtained from the sun-photometer
located near Ersa station
(<uri>http://aeronet.gsfc.nasa.gov/cgi-bin/type_one_station_opera_v2_new</uri>);
the AOD derived at eight wavelengths (from 340 to 1640 nm), the
Ångström exponent (AE) was calculated using the AOD at 440 and
870 nm, and the volume size distribution was retrieved from the algorithm
proposed by <xref ref-type="bibr" rid="bib1.bibx24" id="text.25"/>. The single scattering albedo (SSA)
provides crucial information related to the ratio of scattering to extinction
(scattering plus absorbing) of radiations by aerosols. The sun photometer
data are available several times per day, depending on the solar angle and
aerosol loading <xref ref-type="bibr" rid="bib1.bibx24" id="paren.26"/>. We have also used the aerosol
clear-sky instantaneous direct radiative effect in the shortwave derived from
sun-photometer measurements, following the methodology proposed by
<xref ref-type="bibr" rid="bib1.bibx33" id="text.27"/>. The accuracy of the AERONET retrievals are discussed by
<xref ref-type="bibr" rid="bib1.bibx22" id="text.28"/> and <xref ref-type="bibr" rid="bib1.bibx23" id="text.29"/>.</p>
      <p>Temperature, relative humidity, wind speed and direction measured in
real-time over the whole campaign were taken from the Ersa atmospheric
station. Because the wind measurements may have been influenced by the
orography around the station, we used the wind data provided by the closest
Météo-France station (Semaphore station), which was situated about 5 km away from Ersa and close to the sea. When
the study mentions local wind measurements, it refers to wind observed at the
Semaphore station.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><caption><p>Average mass spectra for fresh and aged sea salt particles observed during ADRIMED.</p></caption>
          <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f01.png"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><caption><p>Scatter plot of TEOM PM<inline-formula><mml:math id="M89" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass concentration as a function of the PM<inline-formula><mml:math id="M90" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> reconstructed mass concentration
for the ADRIMED period.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f02.png"/>

        </fig>

</sec>
<sec id="Ch1.S2.SS2">
  <title>ATOFMS data analysis</title>
      <p>The distinction between aged and fresh sea salt was made according to
the detection of chloride and nitrate in the particles. For fresh sea salt,
we obtained signals for various chloride ions (<inline-formula><mml:math id="M91" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">81</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">83</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>Na<inline-formula><mml:math id="M92" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>Cl<inline-formula><mml:math id="M93" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>,
<inline-formula><mml:math id="M94" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">35</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">37</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>Cl<inline-formula><mml:math id="M95" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> and <inline-formula><mml:math id="M96" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">93</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">95</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>NaCl<inline-formula><mml:math id="M97" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>) and also some nitrate
(<inline-formula><mml:math id="M98" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">46</mml:mn></mml:msup></mml:math></inline-formula>NO<inline-formula><mml:math id="M99" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M100" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">62</mml:mn></mml:msup></mml:math></inline-formula>NO<inline-formula><mml:math id="M101" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>). The signals for chloride are
generally lower for aged sea salt and those for nitrate are stronger due to the
replacement of chloride and sodium nitrate formation <xref ref-type="bibr" rid="bib1.bibx63 bib1.bibx35" id="paren.30"/>. In this case, the relatively small signals for chloride ions
is a good indicator of aged sea salt aerosol. The size distribution of aged
and fresh sea salts was investigated using this differentiation. Regarding
the size distribution, the main limitation is the upper cut-off size of 3
 <inline-formula><mml:math id="M102" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m which limits the detection mostly to fine sea salt particles.</p>
      <p>Average mass spectra for aged and fresh are shown in Fig. <xref ref-type="fig" rid="Ch1.F1"/>. Both
sea salt classes are typical of those observed in other coastal/marine
environments <xref ref-type="bibr" rid="bib1.bibx35 bib1.bibx17 bib1.bibx40" id="paren.31"/>. The positive modes for both fresh and aged particles are
similar and are characterised by sodium ions (<inline-formula><mml:math id="M103" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">23</mml:mn></mml:msup></mml:math></inline-formula>Na<inline-formula><mml:math id="M104" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>,
<inline-formula><mml:math id="M105" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">46</mml:mn></mml:msup></mml:math></inline-formula>Na<inline-formula><mml:math id="M106" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M107" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">62</mml:mn></mml:msup></mml:math></inline-formula>Na<inline-formula><mml:math id="M108" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>O<inline-formula><mml:math id="M109" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>, <inline-formula><mml:math id="M110" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">63</mml:mn></mml:msup></mml:math></inline-formula>Na<inline-formula><mml:math id="M111" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>OH<inline-formula><mml:math id="M112" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> and
<inline-formula><mml:math id="M113" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">81</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">83</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>Na<inline-formula><mml:math id="M114" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>Cl<inline-formula><mml:math id="M115" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>) and <inline-formula><mml:math id="M116" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">39</mml:mn></mml:msup></mml:math></inline-formula>K<inline-formula><mml:math id="M117" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>. The negative mass spectra for
fresh sea salt particles shows peaks for <inline-formula><mml:math id="M118" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">16</mml:mn></mml:msup></mml:math></inline-formula>O<inline-formula><mml:math id="M119" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula>, <inline-formula><mml:math id="M120" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">35</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">37</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>Cl<inline-formula><mml:math id="M121" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula>,
nitrate (<inline-formula><mml:math id="M122" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">46</mml:mn></mml:msup></mml:math></inline-formula>NO<inline-formula><mml:math id="M123" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M124" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">62</mml:mn></mml:msup></mml:math></inline-formula>NO<inline-formula><mml:math id="M125" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>) and
<inline-formula><mml:math id="M126" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">93</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">95</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>NaCl<inline-formula><mml:math id="M127" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>, while the signals for nitrate dominate the aged sea
salt negative mode and sodium chloride adducts are virtually absent. The
occurrence and relative intensity of the chloride and NaCl adducts in ATOFMS
mass spectra are key markers for distinguishing fresh sea salt from aged sea
salt. The absence of NaCl ions and strong nitrate signals indicates extensive
replacement of Cl by NO<inline-formula><mml:math id="M128" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>, while the presence of nitrate in the negative
mass spectra of the fresh sea salt particles suggests that these are not
truly fresh but have also undergone some Cl replacement.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><caption><p>Time series of chemical species (in <inline-formula><mml:math id="M129" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M130" 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>), wind speed (m s<inline-formula><mml:math id="M131" 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 direction (<inline-formula><mml:math id="M132" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>):
<bold>(a)</bold> PMA mass concentration calculated from PILS-IC measurements, <bold>(b)</bold> nss-Ca<inline-formula><mml:math id="M133" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula> mass concentration measured by
PILS-IC measurements, <bold>(c)</bold> nss-NO<inline-formula><mml:math id="M134" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula> mass concentration measured by the PILS-IC, <bold>(d)</bold> nss-SO<inline-formula><mml:math id="M135" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math></inline-formula> mass concentration
measured by the PILS-IC, <bold>(e)</bold> nss-NH<inline-formula><mml:math id="M136" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula> mass concentration measured by the PILS-IC, <bold>(f)</bold> organic mass concentration
measured by the ACSM, <bold>(g)</bold> black carbon mass concentration measured by the MAAP, <bold>(h)</bold> nss-K<inline-formula><mml:math id="M137" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> mass concentration measured
by the PILS-IC, <bold>(i)</bold> PM<inline-formula><mml:math id="M138" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> mass concentration measured by TEOM PM<inline-formula><mml:math id="M139" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula>, <bold>(j)</bold> PM<inline-formula><mml:math id="M140" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass concentration measured by
TEOM PM<inline-formula><mml:math id="M141" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula>, <bold>(k)</bold> wind speed measured at the Semaphore, <bold>(l)</bold> wind direction measured at the Semaphore. The shaded
areas correspond to the three identified periods: orange for dust, blue for primary marine aerosols (PMAs) and brown
for biomass burning/pollution (BBP).</p></caption>
          <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f03.png"/>

        </fig>

</sec>
<sec id="Ch1.S2.SS3">
  <title>FLEXPART model</title>
      <p>We used the FLEXPART Lagrangian dispersion model <xref ref-type="bibr" rid="bib1.bibx87" id="paren.32"/>,
version 9.02. FLEXPART in a backward mode during the campaign to identify the
sources and the transport time of air masses observed at the Ersa station.
The model is driven by wind fields provided by the European Centre for
Medium-Range Weather Forecast (ECMWF) using both analyses and forecasts with
a temporal resolution of 3 h (00:00, 06:00, 12:00, 18:00 h UTC for
analyses and 03:00, 09:00, 15:00, 21:00 h UTC for forecast). The horizontal
resolution is 0.141<inline-formula><mml:math id="M142" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M143" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.141<inline-formula><mml:math id="M144" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> and 91 vertical levels
are used (137 after 25 June 2013). Turbulence is parameterised solving
Langevin equations <xref ref-type="bibr" rid="bib1.bibx86" id="paren.33"/> and the convection
parameterisation scheme is adopted from <xref ref-type="bibr" rid="bib1.bibx26" id="text.34"/> for
all types of convection. The model calculates trajectories of user-defined
ensembles of particles released from a three-dimensional box in backward mode
over 6 days. In this study 10<inline-formula><mml:math id="M145" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msup></mml:math></inline-formula> particles were released at the beginning
of each run in a 100 km <inline-formula><mml:math id="M146" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 160 km <inline-formula><mml:math id="M147" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 200 m
(lat <inline-formula><mml:math id="M148" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> lon <inline-formula><mml:math id="M149" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> alt) box centred above Cap Corse (northern tip
of Corsica). Back trajectories were modelled for three different altitudes:
500 m (bottom and top of the box at 400 and 600 m respectively),
corresponding to the altitude of the measurement site at Ersa; 2000 m,
corresponding to an altitude above the boundary layer; and 4000 m,
corresponding to an altitude where the ATR 42 research aircraft mainly
observed dust plumes <xref ref-type="bibr" rid="bib1.bibx53" id="paren.35"/>. Besides the particles' positions,
FLEXPART also includes cluster analysis for particle ensembles
<xref ref-type="bibr" rid="bib1.bibx88" id="paren.36"/> and the average residence time of particles in
the output grid cells. Cluster analysis uses the plume dispersion information
(residence time) to calculate 10 clusters at each time step (3 h) (using the
k-means clustering), synthesising the particle dispersion information. All
the particles are contained and allocated in these 10 clusters according to
their position (latitude, longitude and altitude; <inline-formula><mml:math id="M150" display="inline"><mml:mi>Z</mml:mi></mml:math></inline-formula>). The horizontal
resolution for the FLEXPART output grid was 1<inline-formula><mml:math id="M151" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M152" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1<inline-formula><mml:math id="M153" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>
and the vertical resolution was 500 m from the ground up to 9500 m.</p>
</sec>
<sec id="Ch1.S2.SS4">
  <title>Aerosol mass closure</title>
      <p>In order to assess the consistency of the chemical data set, we compared
the TEOM PM<inline-formula><mml:math id="M154" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math id="M155" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> data with the online chemical concentration
measurements taken in parallel. PM<inline-formula><mml:math id="M156" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass concentrations were
compared to the sum of chemical components obtained from the PILS-IC
PM<inline-formula><mml:math id="M157" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> data, the BC concentration from the MAAP instrument (PM<inline-formula><mml:math id="M158" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula>),
and the organic matter (OM) concentration derived from the ACSM instrument
(PM<inline-formula><mml:math id="M159" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula>).</p>
      <p>The ratio of the reconstructed mass over the TEOM PM10 mass concentration
averaged 0.79 during the ADRIMED campaign. It is lower during the PMA period
(0.65 <inline-formula><mml:math id="M160" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.20) compared to the BBP period (0.74 <inline-formula><mml:math id="M161" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.23). We did not
measure TEOM PM10 during the dust period. We did not find any significant
correlation between missing mass and TEOM PM10 mass, even though the missing
mass is globally higher when the PM10 total mass is higher. This lack of
aerosol mass could also be due to the mass of (insoluble) dust not determined
chemically or possibly a supermicron mode of organic that was not determined
here. Indeed, the organic mass fraction can represent more than 10 % of the
sea spray mass for aerosols between 1 and 3 <inline-formula><mml:math id="M162" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m during a period of
high biological activity <xref ref-type="bibr" rid="bib1.bibx31" id="paren.37"/>. This ratio decreases
with increasing size. Even though full mass closure has not been reached,
there is no impact on the results because the losses do not represent sources
by themselves. The three main aerosol types presented in this paper have
been determined using key chemical tracers (measured by the PILS and ACSM),
optical properties (MAAP and nephelometer), FLEXPART back-trajectory analysis
for confirmation. The combination of these different analyses conducted in
this study is found to be coherent and representative of the whole aerosol
population.</p>
      <p>For this study, the sulfate (SO<inline-formula><mml:math id="M163" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math></inline-formula>) and NH<inline-formula><mml:math id="M164" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula> data were taken
from the PILS-IC instrument as the correlation between ACSM and PILS-IC
measurements show a very good agreement (SO<inline-formula><mml:math id="M165" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math></inline-formula>(PILS) <inline-formula><mml:math id="M166" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 0.99 <inline-formula><mml:math id="M167" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> SO<inline-formula><mml:math id="M168" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math></inline-formula>(ACSM)), <inline-formula><mml:math id="M169" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.95</mml:mn></mml:mrow></mml:math></inline-formula> and
NH<inline-formula><mml:math id="M170" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>(PILS) <inline-formula><mml:math id="M171" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 1.27 <inline-formula><mml:math id="M172" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> NH<inline-formula><mml:math id="M173" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>(ACSM), <inline-formula><mml:math id="M174" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.8</mml:mn></mml:mrow></mml:math></inline-formula>7).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><caption><p>Correlation plot of chemical components mass concentrations, PM<inline-formula><mml:math id="M175" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math id="M176" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass
concentration and wind speed and direction, over the whole campaign.</p></caption>
          <?xmltex \igopts{width=321.516142pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f04.png"/>

        </fig>

</sec>
</sec>
<sec id="Ch1.S3">
  <title>Results</title>
<sec id="Ch1.S3.SS1">
  <title>Overview of aerosols sources</title>
      <p>In this section, the chemical properties of the aerosols measured in Ersa
(Fig. <xref ref-type="fig" rid="Ch1.F3"/>) are first studied, revealing a significant variability in
the contribution of the different aerosol species and outlining three main
periods, dust, PMA and BBP, under the influence of different types of air
masses and particles. The aerosol physical properties are then discussed in
Sect. 3.2.3 and 3.3.1.</p>
      <p><?xmltex \hack{\newpage}?>The mean PM<inline-formula><mml:math id="M177" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> concentration measured by the TEOM PM<inline-formula><mml:math id="M178" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> during the
ADRIMED campaign was 11.5 <inline-formula><mml:math id="M179" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 5.4 <inline-formula><mml:math id="M180" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M181" 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 majority of the
sampling period the mass concentration ranged from 10 to 20 <inline-formula><mml:math id="M182" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M183" 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>,
except for short periods when the concentration fell to 5 <inline-formula><mml:math id="M184" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M185" 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 decreases are usually due to wet scavenging or the diurnal variation
of the boundary layer, as the Ersa station was within the boundary layer
during daytime and sometimes slightly above the boundary layer at
night-time (aerosol concentrations at night were often lower when the Ersa
site was in the free troposphere).
In parallel, the mean PM<inline-formula><mml:math id="M186" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> concentration measured by the TEOM PM<inline-formula><mml:math id="M187" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> during ADRIMED was 6.4 <inline-formula><mml:math id="M188" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3.2 <inline-formula><mml:math id="M189" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M190" 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 concentration was lower during June and rises during the beginning of July to exceed 10 <inline-formula><mml:math id="M191" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M192" 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 major chemical constituents of PM<inline-formula><mml:math id="M193" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> measured at Ersa (Fig. <xref ref-type="fig" rid="Ch1.F3"/>) show a significant temporal variability during the campaign. A
correlation plot (Fig. <xref ref-type="fig" rid="Ch1.F4"/>) illustrates the relationship
between the principal chemical constituents, PM<inline-formula><mml:math id="M194" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math id="M195" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass
concentrations, as well as wind speed and direction. In the figure, the order
of the variables appear due to their similarity with one another, through
hierarchical analysis <xref ref-type="bibr" rid="bib1.bibx10" id="paren.38"/>. The colour and the number
represent the correlation between two variables: when close to 100, the
correlation is high. The shape of the ellipse is a visual representation of a
scatter plot. We can observe two groups of variables on this figure. The first
one is composed of Cl<inline-formula><mml:math id="M196" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula>, Na<inline-formula><mml:math id="M197" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula>, Ca<inline-formula><mml:math id="M198" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula>, K and PM<inline-formula><mml:math id="M199" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass
concentration and related to marine or terrestrial influence, while the second
one, composed of NH<inline-formula><mml:math id="M200" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>, SO<inline-formula><mml:math id="M201" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math></inline-formula>, BC, organics and PM<inline-formula><mml:math id="M202" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> mass
concentration, is related to pollution influence.
Three main periods under the influence of different types of air masses and aerosols have been selected here and discussed in more details below.</p>
      <p>The first period (16 to 20 June) corresponds to a dust outbreak and is
characterised by the concentration of non-sea-salt calcium (nss-Ca<inline-formula><mml:math id="M203" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula>)
concentration, a proxy of desert dust <xref ref-type="bibr" rid="bib1.bibx78" id="paren.39"/>, which increases
from 0.5 to 2 <inline-formula><mml:math id="M204" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M205" 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>. This dust event lasted a few days, from 16 to
20 June, with nss-Ca<inline-formula><mml:math id="M206" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula> concentrations peaking on 18 June at 2 <inline-formula><mml:math id="M207" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M208" 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> at the Ersa site. In addition, the concentrations of calcium
measured by the PILS-IC are relatively low for a dust event, because the
maximum concentration of dust particles was located at an altitude ranging
between 3 and 6 km <xref ref-type="bibr" rid="bib1.bibx18" id="paren.40"/>. The second reason concerns the
method used by the PILS-IC instrument, which analyses only the soluble fraction
of aerosols, while a significant part of dust Ca is insoluble. In that sense,
the concentration of nss-Ca<inline-formula><mml:math id="M209" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula> determined by PILS-IC remains a
qualitative indicator of the presence of dust particles.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><caption><p>Ratio of inorganic sea salt mass concentration (PILS-IC) over PM<inline-formula><mml:math id="M210" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula>
mass concentration (TEOM PM<inline-formula><mml:math id="M211" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula>).</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f05.png"/>

        </fig>

      <p>PILS-IC measurements also indicate an increase in the concentrations of
oxalate, potassium, SO<inline-formula><mml:math id="M212" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math></inline-formula> and NH<inline-formula><mml:math id="M213" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula> from 5 to 9 July, which
correspond to BBP influences. A brief increase of NO<inline-formula><mml:math id="M214" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>
concentrations (PILS-IC) was recorded on 5 and 6 July (Fig. <xref ref-type="fig" rid="Ch1.F3"/>).
This event was also detected by the ACSM. Indeed, there is a difference of a factor of 2 in terms of total mass concentrations
between the first part of the campaign (6 June to 4 July) and during the BBP period. During the first period (6 June to 4 July),
the mass concentration of each aerosol species is low, characterised by a mean total concentration of
3.7 <inline-formula><mml:math id="M215" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.6 <inline-formula><mml:math id="M216" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M217" 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>. During the second identified period (4 to 13 July), the total PM<inline-formula><mml:math id="M218" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula>
aerosol mass concentration increases suddenly to reach a mean of 7.2 <inline-formula><mml:math id="M219" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.7 <inline-formula><mml:math id="M220" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M221" 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>. Similarly,
the total PM1 mass concentration measured by the TEOM increases from 5.9 <inline-formula><mml:math id="M222" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3.0 to 8.4 <inline-formula><mml:math id="M223" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3.3 <inline-formula><mml:math id="M224" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M225" 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>.
This increase is mainly due to a large addition of the concentration of submicronic organics compounds
(from 2.1 <inline-formula><mml:math id="M226" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.9 <inline-formula><mml:math id="M227" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M228" 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> to 4.1 <inline-formula><mml:math id="M229" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.2 <inline-formula><mml:math id="M230" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M231" 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 an increase
of SO<inline-formula><mml:math id="M232" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math></inline-formula> (and NH<inline-formula><mml:math id="M233" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula>) from 0.9 <inline-formula><mml:math id="M234" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.6 (0.5 <inline-formula><mml:math id="M235" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.3) to 1.8 <inline-formula><mml:math id="M236" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.6 (0.9 <inline-formula><mml:math id="M237" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.3) <inline-formula><mml:math id="M238" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M239" 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>.
organics, sulfate and ammonium concentrations remain high until 10 July, when they decrease, but to values that are still higher than
during the month of June. In parallel, the black carbon (BC) concentration is found to be low throughout the whole period of the campaign,
although we observe an increase during July (mean of 0.41 <inline-formula><mml:math id="M240" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11 <inline-formula><mml:math id="M241" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M242" 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>) compared to June
(mean of 0.28 <inline-formula><mml:math id="M243" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11 <inline-formula><mml:math id="M244" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M245" 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 a few days and during the PMA period, the concentration of BC is
found to be very low (0.20 <inline-formula><mml:math id="M246" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09 <inline-formula><mml:math id="M247" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M248" 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 recovers its previous concentration by 3 July.
The highest BC concentration (0.75 <inline-formula><mml:math id="M249" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M250" 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>) was reached on 5 July. The ACSM observations clearly
indicate that concentrations of all the chemical components during the BBP episode are twice the concentration they
had during the first period of the ADRIMED campaign. Similar episodes of biomass burning events of European origin
were studied by <xref ref-type="bibr" rid="bib1.bibx73" id="text.41"/> at a Mediterranean site, with an increase in the concentration of PM<inline-formula><mml:math id="M251" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula>
nitrate (6 times higher than the annual average), sulfate (about 3 times higher than the annual average), ammonium (more than
4 times higher than the annual average), OM (about 2 times higher than the annual average) and potassium (2 times higher than the annual average).</p>
      <p>Our observations reveal that the mean concentration of inorganic PMA
(averaged for the months of June and July 2013) was found to be low with a
value of 0.76 <inline-formula><mml:math id="M252" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.04 <inline-formula><mml:math id="M253" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M254" 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> (Fig. <xref ref-type="fig" rid="Ch1.F3"/>). However, during
the PMA period, the concentration of PMA increases up to 6.5 <inline-formula><mml:math id="M255" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M256" 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>,
with a mean concentration of 3.2 <inline-formula><mml:math id="M257" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.8 <inline-formula><mml:math id="M258" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M259" 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 this specific
period, the mass of PMA represents, on average, 22 % of the total mass
measured by the TEOM PM<inline-formula><mml:math id="M260" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> instrument, while the average contribution was
about 7 % for the whole period of observations. At the Ersa station, the
highest concentration of PMA was reached on 24 June, when PMA concentration
represented 40 % of hourly PM<inline-formula><mml:math id="M261" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass concentration for 25 % of the data
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>). Even though the mean values of PMA mass
concentration measured at Ersa were low compared to values referenced at
other Mediterranean sites, this contribution still remains significant.
Indeed, Pey et al. (2009) reported a ratio of 10 % of sea spray (sum of Na
and Cl<inline-formula><mml:math id="M262" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> mass concentrations from Quartz fibre filter) to PM<inline-formula><mml:math id="M263" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula>
(annual mean <inline-formula><mml:math id="M264" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 2.9 <inline-formula><mml:math id="M265" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M266" 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 Mallorca (117 m a.s.l.), while
<xref ref-type="bibr" rid="bib1.bibx5" id="text.42"/> found a contribution of 40 % of PMA in the coarse mode
of inorganic ions during summer at Finokalia (150 m a.s.l., Crete).
<xref ref-type="bibr" rid="bib1.bibx69" id="text.43"/> analysed the chemical composition of PM<inline-formula><mml:math id="M267" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> aerosols in
the Mediterranean Basin and found a mean annual contribution of sea spray to
PM<inline-formula><mml:math id="M268" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> that did not exceed 24 %. So the contribution of inorganic sea salt
to the PM<inline-formula><mml:math id="M269" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass concentration in the Mediterranean Basin is on average
lower than 20 % but can reach 40 % during particular events such as the one
observed at Ersa in June 2013. Moreover, sea spray likely comprises a
substantial fraction of organic PMA and hence may represent a larger fraction
of PM<inline-formula><mml:math id="M270" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> than the one estimated solely from the inorganic fraction
<xref ref-type="bibr" rid="bib1.bibx31" id="paren.44"/>. Furthermore, while the contribution of PMA to
PM<inline-formula><mml:math id="M271" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass concentration is high during the PMA period, the mass contribution
of nss ions to the total ionic content is relatively low during the PMA
period (53 <inline-formula><mml:math id="M272" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 11 %). In comparison, the mass contribution of nss-ions to
the total ionic content is 84 <inline-formula><mml:math id="M273" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 5 % for the ADRIMED field campaign, and
is 82 <inline-formula><mml:math id="M274" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 14 and 92 <inline-formula><mml:math id="M275" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3 % for the dust and BBP periods
respectively. Furthermore, the Ca<inline-formula><mml:math id="M276" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula> concentration measured during the
PMA period (up to 2 <inline-formula><mml:math id="M277" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M278" 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>) indicates the presence of dust
particles, probably related to strong winds lifting soil/dust in the vicinity
of the Ersa station <xref ref-type="bibr" rid="bib1.bibx4" id="paren.45"/>. However, unlike the dust period, they
do not represent the dominant aerosol influence during the PMA period.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><caption><p>Maps representing the different zones used for the study of the origin of air masses
with FLEXPART. <bold>(a)</bold> Anthropogenic and desert zones (red for Spanish coasts, dark blue for French coasts,
green for Italy, blue for Greece, orange and yellow for northern Africa. <bold>(b)</bold> Marine zones
(G corresponds to Gulf of Lion, B to Bay of Biscay).</p></caption>
          <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f06.png"/>

        </fig>

      <p>However, unlike the dust period (16–20 June), the major aerosol influence
during the PMA period is PMA, with a mass concentration reaching 6.5 <inline-formula><mml:math id="M279" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M280" 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>, which is 3 times higher than nss-Ca<inline-formula><mml:math id="M281" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>+</mml:mo></mml:mrow></mml:msup></mml:math></inline-formula> mass concentration.
Indeed, during the dust period, PMA mass concentration is low (0.4 <inline-formula><mml:math id="M282" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.3 <inline-formula><mml:math id="M283" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M284" 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 so the main aerosol mass contribution are dust
particles.</p>
<sec id="Ch1.S3.SS1.SSS1">
  <title>Origins and time of residence of the different air-masses observed at Ersa</title>
      <p>The origin of air masses impacting Ersa for the three different periods
depicted in Fig. <xref ref-type="fig" rid="Ch1.F3"/> has been investigated using FLEXPART model in
order to characterise the transport time and the emitting sources of these
aerosols.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><caption><p>Time series of air mass sources derived from the FLEXPART back-trajectory simulations at
500 m from 7 June 2013 to 13 July 2013. The top panel <bold>(a)</bold> represents the passage of an air mass through the
different zones before they reached Ersa. Panel <bold>(b)</bold> represents the transport time of the air masses from each
zone in <bold>(a)</bold> to Ersa.</p></caption>
            <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f07.png"/>

          </fig>

      <p>Figure <xref ref-type="fig" rid="Ch1.F7"/>a represents the time series computed from
clusters of FLEXPART back trajectories. The upper one represents the transport of
the air masses passing over different regions before reaching the Ersa
station. These different zones take into account the regions influenced by
anthropogenic pollution, biomass burning and marine influences and are
represented in Fig. <xref ref-type="fig" rid="Ch1.F6"/>. They represent the most probable influence
on air masses arriving in Cap Corse due to their close locations and
specific emissions. For each day during the campaign (bottom axes), the upper
figure indicates the different zones through which the air masses passed
before reaching Ersa. The bottom figure indicates the transport time from
these zones to the Ersa sample site.</p>
      <p>In general, the Ersa station was influenced by air masses coming from the west
and south during the first part of the field campaign (from 6 to 26 June),
and was more influenced by air masses coming from the east and north during the
last part of the campaign (26 June to 13 July). During the campaign, Ersa was
always affected by air masses that passed over French or Italian coastal
areas. The influence of the Mediterranean coasts of Spain is also very
present during the campaign, especially in the first part of June.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8" specific-use="star"><caption><p>FLEXPART maps representing for <bold>(a, b, c)</bold> the probability density of the back trajectories for the three periods: dust, PMA and BBP. The bottom panels <bold>(d, e, f)</bold> represent
the mean transport time from the Ersa station for the three periods: dust, PMA and BBP. Each
back trajectory starts at 500 m from the Ersa measurement site.</p></caption>
            <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f08.png"/>

          </fig>

      <p>In terms of transport time, FLEXPART simulations indicate that air masses
spent a few hours to several days over the sea after leaving the French or
Italian coasts, and 2 to 6 days from continental European sources.
Coastal regions are likely the source of anthropogenic-pollution impacted air
masses, because they are highly industrialised and populated and are the last
major source of anthropogenic aerosols before transport over the
Mediterranean Sea. At the local scale, Ersa was mostly under the influence of
a westerly wind (<inline-formula><mml:math id="M285" display="inline"><mml:mo>≃</mml:mo></mml:math></inline-formula> 270<inline-formula><mml:math id="M286" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>; Fig. <xref ref-type="fig" rid="Ch1.F3"/>) from the
beginning of the campaign to the beginning of July, expect for a few days
during the dust outbreak (from 16 to 20 June), where it was under a
south-eastern influence (<inline-formula><mml:math id="M287" display="inline"><mml:mo>≃</mml:mo></mml:math></inline-formula> 150<inline-formula><mml:math id="M288" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>). Finally, from 4 to 9 July,
Ersa was mostly experiencing an easterly wind (<inline-formula><mml:math id="M289" display="inline"><mml:mo>≃</mml:mo></mml:math></inline-formula> 100<inline-formula><mml:math id="M290" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>).</p>
      <p>The influence of southerly air masses is marked by the passage of air masses
above northern Africa, at the beginning of the campaign (19 June, Fig. <xref ref-type="fig" rid="Ch1.F8"/>). The transport time of air masses from northern Africa to
Ersa ranges between 2 and 6 days. Such air masses contain significant
concentrations of mineral dust particles, which are usually transported at
higher altitudes over the Mediterranean Basin, in the free troposphere and up
to 9 km in altitude <xref ref-type="bibr" rid="bib1.bibx18 bib1.bibx39 bib1.bibx25 bib1.bibx20 bib1.bibx58 bib1.bibx36" id="paren.46"/>. Thus, we
also performed simulations starting at 4000 m a.s.l., that show that the air
masses arriving at Cap Corse on 19 and 20 June were within the boundary
layer (<inline-formula><mml:math id="M291" display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 1000 m) over Tunisia and Algeria from 2 to 3 days before. At the
Ersa site, during the dust outbreak around 19 June, the wind speed reached
15 m s<inline-formula><mml:math id="M292" 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>.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><caption><p>Transport time (mean <inline-formula><mml:math id="M293" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> standard deviation) from the Gulf of Lion and North Atlantic Ocean to the Ersa station
obtained from FLEXPART simulations analyses (see Sect. 3.1.1).</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="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">22 June</oasis:entry>  
         <oasis:entry colname="col3">23 June</oasis:entry>  
         <oasis:entry colname="col4">24 June</oasis:entry>  
         <oasis:entry colname="col5">25 June</oasis:entry>  
         <oasis:entry colname="col6">26 June</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">Gulf of Lion: mean transport time</oasis:entry>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3"/>  
         <oasis:entry colname="col4"/>  
         <oasis:entry colname="col5"/>  
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">(days)</oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math id="M294" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.72</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">0.69</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3"><inline-formula><mml:math id="M295" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.49</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.29</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col4"><inline-formula><mml:math id="M296" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.21</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">0.09</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5"><inline-formula><mml:math id="M297" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.55</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">0.30</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col6"><inline-formula><mml:math id="M298" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.32</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">0.50</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">North Atlantic Ocean: mean transport time</oasis:entry>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3"/>  
         <oasis:entry colname="col4"/>  
         <oasis:entry colname="col5"/>  
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">(days)</oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math id="M299" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.88</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">0.87</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3"><inline-formula><mml:math id="M300" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.50</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.72</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col4"><inline-formula><mml:math id="M301" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.94</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">1.5</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5"><inline-formula><mml:math id="M302" display="inline"><mml:mrow><mml:mn mathvariant="normal">3.23</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">1.26</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col6"><inline-formula><mml:math id="M303" display="inline"><mml:mrow><mml:mn mathvariant="normal">4.45</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">1.22</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p>Besides the coastal anthropogenic influence observed during the first week of
July, Fig. <xref ref-type="fig" rid="Ch1.F8"/> shows that the air masses came from eastern
Europe from 7 to 12 July, and in particular from Ukraine, 3–4 days before reaching
Ersa. The date at which the air masses passed over these regions corresponds
to significant emissions of biomass burning observed near the Black Sea as
shown by the MODIS satellite retrievals
(<uri>http://rapidfire.sci.gsfc.nasa.gov/cgi-bin/imagery/firemaps.cgi</uri>).</p>
      <p>FLEXPART back-trajectory simulations also show that during the PMA period,
air masses were coming from the north-west of Cap Corse, including the Gulf of
Lion. This is consistent with a higher PMA concentration in Ersa, as a longer
fetch leads to higher mass concentration. Our simulations reveal that these
air masses were also influenced by anthropogenic sources from France and
Italy. The study of the transport of air masses passing over maritime zones
(Fig. <xref ref-type="fig" rid="Ch1.F7"/>b), especially the Gulf of Lion and North Atlantic
zones, gives us information about the transport time from the source regions
to Ersa and the changes in altitude. Our simulations indicate that the mean transport
time from the Gulf of Lion is less than a day for the whole period except for
the last day, 26 June. Whereas from the North Atlantic zone (Bay of Biscay),
the transport time is more than 2.5 days and increases up to 4.5 days for 26 June (Table <xref ref-type="table" rid="Ch1.T1"/>). Almost no precipitation occurred
during this period between the Bay of Biscay and Corsica, so these air masses
were likely not impacted by wet scavenging.</p>
      <p>The mean altitude for the air masses coming from the Gulf of Lion is close to
1000 m (972 m <inline-formula><mml:math id="M304" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 753) for the 5 days, with minima mainly below 500 m,
while the mean altitude from the North Atlantic is 1374 m (<inline-formula><mml:math id="M305" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>828) and the
minimum is below 800 m only for the first 3 days. <xref ref-type="bibr" rid="bib1.bibx91" id="text.47"/>
reported that the concentration of sea salt aerosols associated with emissions
was highest up to altitudes of 600–700 m, which typically correspond to the
marine boundary layer (MBL) height. Thus an influence from the North Atlantic
Ocean would occur more likely during the first 3 days of the period, when the
air masses lay within the MBL. Concerning the Gulf of Lion, the altitudes of
the air masses are low enough to bring sea salt aerosols in Ersa. While
vertical transport is not well captured in the model, the FLEXPART model
indicates that most of the PMA aerosol mass is transported in the MBL.</p>
      <p>To summarise, our FLEXPART simulations clearly indicate that the Ersa site
was impacted by a disperse set of air masses from different regions
transporting different types of aerosols. These FLEXPART results are
consistent with chemical measurements obtained at Ersa station, as well as
the three periods discussed here.</p>
      <p>The following sections will focus on the optical, physical and chemical
properties of aerosols sampled during the PMA period. The dust and BBP events
will be used as a comparison for different states of the atmosphere impacting
the Ersa site.</p>
</sec>
</sec>
<sec id="Ch1.S3.SS2">
  <title>Primary marine aerosols</title>
<sec id="Ch1.S3.SS2.SSS1">
  <title>PMA ageing</title>
      <p>As reported by <xref ref-type="bibr" rid="bib1.bibx12" id="text.48"/> and <xref ref-type="bibr" rid="bib1.bibx71" id="text.49"/>, the ratio of
the concentration of Cl<inline-formula><mml:math id="M306" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> over Na<inline-formula><mml:math id="M307" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> is an indicator of the chloride
depletion that happens when PMAs react with acidic gases like HNO<inline-formula><mml:math id="M308" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and
H<inline-formula><mml:math id="M309" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>SO<inline-formula><mml:math id="M310" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:math></inline-formula> according to the chemical Reactions (R1, R2, R3):</p>
      <p>

                  <disp-formula specific-use="align" content-type="numbered reaction"><mml:math id="M311" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="Ch1.E1"><mml:mtd/><mml:mtd><mml:mstyle class="stylechange" displaystyle="true"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:mn mathvariant="normal">2</mml:mn><mml:mi mathvariant="normal">NaCl</mml:mi></mml:mrow><mml:mo>→</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">Na</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:mn mathvariant="normal">2</mml:mn><mml:mi mathvariant="normal">HCl</mml:mi></mml:mrow></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E2"><mml:mtd/><mml:mtd><mml:mstyle class="stylechange" displaystyle="true"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mrow class="chem"><mml:mi mathvariant="normal">NaCl</mml:mi></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow><mml:mo>→</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NaHSO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">HCl</mml:mi></mml:mrow></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E3"><mml:mtd/><mml:mtd><mml:mstyle class="stylechange" displaystyle="true"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mrow class="chem"><mml:mi mathvariant="normal">NaCl</mml:mi></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">HNO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>→</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">HCl</mml:mi></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NaNO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula></p>
      <p>These reactions result in a loss of particulate chloride in PMAs during
transport. The typical mass ratio of Cl<inline-formula><mml:math id="M312" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M313" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula> Na<inline-formula><mml:math id="M314" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> of the sea water is
1.8 <xref ref-type="bibr" rid="bib1.bibx49" id="paren.50"/>; however, the study of PM<inline-formula><mml:math id="M315" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> PMA in the
Mediterranean Basin by <xref ref-type="bibr" rid="bib1.bibx77" id="text.51"/> shows a Cl<inline-formula><mml:math id="M316" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M317" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula> Na<inline-formula><mml:math id="M318" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> ratio of
1.2. Numerous values are referenced over the Mediterranean Basin: 0.6 for
long-term measurements (July 2012–April 2013) in Ersa station
<xref ref-type="bibr" rid="bib1.bibx62" id="paren.52"/>, 0.49 by <xref ref-type="bibr" rid="bib1.bibx56" id="text.53"/>, 1.00 by
<xref ref-type="bibr" rid="bib1.bibx47" id="text.54"/>, 1.2 during summer by <xref ref-type="bibr" rid="bib1.bibx5" id="text.55"/> in
Finokalia (eastern Mediterranean, Crete) and 1.2 during summer in the
eastern Mediterranean coast of Turquey by <xref ref-type="bibr" rid="bib1.bibx46" id="text.56"/>. These values are
found to be low compared to the seawater ratio, especially those by
<xref ref-type="bibr" rid="bib1.bibx56" id="text.57"/>, which is probably related to the high reactivity of chloride
with acidic gases that are present in relatively high concentrations in the
Mediterranean atmosphere <xref ref-type="bibr" rid="bib1.bibx81 bib1.bibx5 bib1.bibx68" id="paren.58"/>. A good
correlation was found between Na<inline-formula><mml:math id="M319" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> mass concentration and the sum of
Cl<inline-formula><mml:math id="M320" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M321" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> NO<inline-formula><mml:math id="M322" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula> mass concentrations (PM10 measurements; <inline-formula><mml:math id="M323" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.87</mml:mn></mml:mrow></mml:math></inline-formula>) indicating that NO<inline-formula><mml:math id="M324" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn><mml:mo>-</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula> is the main component that interacts with sea
salt.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9"><caption><p>Comparison of the two instruments ATOFMS and PILS-IC for inorganic component of sea salt aerosols.
The time series represents the mass ratio of chloride to sodium ions calculated from the PILS-IC measurements.
The marker colour represents the degree of ageing determined by the ATOFMS.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f09.png"/>

          </fig>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T2"><caption><p>Characteristics of the three log-normal modes of aged sea salt aerosols measured by ATOFMS at Ersa station</p></caption><oasis:table frame="topbot"><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>  
         <oasis:entry colname="col1">Mode</oasis:entry>  
         <oasis:entry colname="col2">Aerodynamical</oasis:entry>  
         <oasis:entry colname="col3"><inline-formula><mml:math id="M325" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">diameter <inline-formula><mml:math id="M326" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m</oasis:entry>  
         <oasis:entry colname="col3"/>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">1</oasis:entry>  
         <oasis:entry colname="col2">0.46</oasis:entry>  
         <oasis:entry colname="col3">1.28</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">2</oasis:entry>  
         <oasis:entry colname="col2">1.13</oasis:entry>  
         <oasis:entry colname="col3">1.35</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">3</oasis:entry>  
         <oasis:entry colname="col2">1.95</oasis:entry>  
         <oasis:entry colname="col3">1.23</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p>During the PMA period, the Cl<inline-formula><mml:math id="M327" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M328" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula> Na<inline-formula><mml:math id="M329" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> mass ratio varies between 0.13 and
1.3 (Fig. <xref ref-type="fig" rid="Ch1.F9"/>), with a mean of 0.59 <inline-formula><mml:math id="M330" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.23. This result is
consistent with the long-term measurement taken between July 2012 and
April 2013 at Ersa <xref ref-type="bibr" rid="bib1.bibx62" id="paren.59"/>. This indicates that
PMA measured in Ersa (and throughout the Mediterranean Basin) were
predominantly aged.</p>
      <p>To distinguish mostly aged and mostly fresh PMA, we used a spectral
analysis of the ATOFMS measurements. The terms “fresh” and “aged” PMA, which will
be used from now in this text correspond to the classification made with the
ATOFMS. During the ChArMEx-ADRIMED campaign, an alternation between these two
states of PMA was detected.</p>
      <p>The size distribution of these two ATOFMS sea salt types were fitted
according to a sum of log-normal modes. The fresh PMA were characterised by
one mode with a vacuum aerodynamic diameter of 1.29 <inline-formula><mml:math id="M331" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and a standard
deviation <inline-formula><mml:math id="M332" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> of 1.34, while the aged PMA were characterised by three
different modes, as detailed in Table <xref ref-type="table" rid="Ch1.T2"/>.</p>
      <p>Our results show that during the campaign aged PMA are dominant, but during
the PMA period (22–26 June) when the wind near Cap Corse is higher (Sect. 3.2.2), there is an alternation of short events of fresh or aged PMA, with a
dominance of fresh PMA. The comparison of the ATOFMS and PILS data show a
relatively good agreement between the two instruments regarding the dominance
of fresh and aged PMA (Fig. <xref ref-type="fig" rid="Ch1.F9"/>).</p>
      <p>To compare the two instruments, we looked at the count ratio of aged to fresh PMA,
and attributed a state to the Cl<inline-formula><mml:math id="M333" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M334" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula> Na<inline-formula><mml:math id="M335" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> ratio measured by the
PILS-IC. For a large number of measurements only aged aerosols were detected
and were labelled “only aged”. When the count ratio of aged aerosols
over fresh aerosols was higher than one, the measurements were characterised
as mostly aged, and less than one the PMA were considered mostly fresh.
One can observe in Fig. <xref ref-type="fig" rid="Ch1.F9"/> that the Cl<inline-formula><mml:math id="M336" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M337" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula> Na<inline-formula><mml:math id="M338" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> ratio is
higher when the ATOFMS distinguished fresh PMA, and lower when the ATOFMS
distinguished aged PMA. We then determined the mean Cl<inline-formula><mml:math id="M339" display="inline"><mml:msup><mml:mi/><mml:mo>-</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M340" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula> Na<inline-formula><mml:math id="M341" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> ratio
for mostly aged (0.38 <inline-formula><mml:math id="M342" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.15) and mostly fresh PMA (0.62 <inline-formula><mml:math id="M343" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.17). In
our observations, the mostly fresh PMA ratio remains low compared to the
initial ratio of 1.8 <xref ref-type="bibr" rid="bib1.bibx49" id="paren.60"/> or even 1.2 for PM<inline-formula><mml:math id="M344" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> PMA
(Schwier et al., 2016), revealing that even though PMA are characterised as
fresh, they have undergone chemical reactions before reaching Ersa station.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F10" specific-use="star"><caption><p>PMA concentration measured at Ersa as a function of wind speed for the ADRIMED period. The PMA concentrations
have been averaged by wind speed bins of 1 m s<inline-formula><mml:math id="M345" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. The error bars represent <inline-formula><mml:math id="M346" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 2<inline-formula><mml:math id="M347" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>/<inline-formula><mml:math id="M348" display="inline"><mml:msqrt><mml:mi>N</mml:mi></mml:msqrt></mml:math></inline-formula> (<inline-formula><mml:math id="M349" display="inline"><mml:mi>N</mml:mi></mml:math></inline-formula> is the
number of independent measurements). <bold>(a)</bold> The black curve correspond to measurements, while the red, blue and green
curves correspond to fits parameters by <xref ref-type="bibr" rid="bib1.bibx7 bib1.bibx90 bib1.bibx54" id="text.61"/>.
Panel <bold>(b)</bold> represents fresh (blue curve) and aged (red curve) PMA over the whole campaign.</p></caption>
            <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f10.png"/>

          </fig>

</sec>
<sec id="Ch1.S3.SS2.SSS2">
  <title>PMA sources</title>
      <p>Complementary to the FLEXPART results, we used wind measurements at the
Semaphore station, at the Gulf of Lion buoy and at the Bay of Biscay buoy to
investigate the possible relationship between the increase in PMA
concentration observed in Ersa and the wind speed at these stations, as well
as to better assess the origin of sea salt aerosols at Ersa.</p>
      <p>During the ChArMEx-ADRIMED campaign, the majority of analysed air masses
containing PMA came locally from the west and the concentration of
marine particles increased with wind speed (Fig. <xref ref-type="fig" rid="Ch1.F10"/>a). The wind
direction is constant around 270<inline-formula><mml:math id="M350" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> for 6 days (21–26 June), and
fluctuates afterwards between eastern and western origins. The maximum wind speed
(20 m s<inline-formula><mml:math id="M351" 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>) encountered during the campaign was observed on 24 June,
coinciding with the highest sea salt mass concentration measured.</p>
      <p>To investigate the relationship between wind speed and concentration of PMA
measured in Ersa, we averaged its concentration by wind bins of 1 m s<inline-formula><mml:math id="M352" 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 different cases. We first looked at the relationship between the
concentration of PMA in Ersa and the wind speed measured at the Semaphore for
the whole period of the campaign (Fig. <xref ref-type="fig" rid="Ch1.F10"/>a). The result indicates
a relationship between the wind speed and PMA concentration and the best fit
(<inline-formula><mml:math id="M353" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.92</mml:mn></mml:mrow></mml:math></inline-formula>) is presented in the form of ln [PMA] <inline-formula><mml:math id="M354" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> <inline-formula><mml:math id="M355" display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M356" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> WS <inline-formula><mml:math id="M357" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> ln(<inline-formula><mml:math id="M358" display="inline"><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>), where WS corresponds to the wind speed and <inline-formula><mml:math id="M359" display="inline"><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M360" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M361" 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>)
to the concentration that corresponds to a wind speed WS <inline-formula><mml:math id="M362" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 0. The error bars
correspond to 2<inline-formula><mml:math id="M363" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> rms (root mean square). Above 13 m s<inline-formula><mml:math id="M364" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, the
concentration starts to rise rapidly. The relationship described here is
compared with fit parameters found by <?xmltex \hack{\mbox\bgroup}?><xref ref-type="bibr" rid="bib1.bibx7" id="text.62"/><?xmltex \hack{\egroup}?>,
<xref ref-type="bibr" rid="bib1.bibx90 bib1.bibx54 bib1.bibx49" id="text.63"/> and chosen
because the time resolution of the measurements were similar to those in Ersa
and wind speed encountered during their measurements were in the same
range as in Ersa during the campaign. Despite the high correlation between
PMA concentration and wind speed shown here, our results yield mass
concentrations at least an order of magnitude lower than other studies shown
in Fig. <xref ref-type="fig" rid="Ch1.F10"/>. This difference is probably related to the sampling
altitudes, which for our study was 533, and <inline-formula><mml:math id="M365" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 10 m a.s.l. for <xref ref-type="bibr" rid="bib1.bibx7 bib1.bibx90" id="text.64"/> and
<xref ref-type="bibr" rid="bib1.bibx54" id="text.65"/>. This is contrary to <xref ref-type="bibr" rid="bib1.bibx27" id="text.66"/>, who did
not find a significant correlation between PMA concentrations and wind speed
in Cabo Verde, even though they found an increase of PMA concentration on days
of higher wind speeds.
<xref ref-type="bibr" rid="bib1.bibx81" id="text.67"/> had difficulties establishing a relationship between local emissions of PMA and wind speed measurements using
instrumentation with a long integration time during the FETCH campaign, in accordance with previous results of
<xref ref-type="bibr" rid="bib1.bibx70" id="text.68"/>. <xref ref-type="bibr" rid="bib1.bibx82" id="text.69"/> found that wind speed was a good indicator for a measuring period but not for a specific case.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F11" specific-use="star"><caption><p>Concentration of sea salt aerosols measured by the PILS IC as a function of wind speed measured at
Ersa <bold>(a)</bold>, at the Gulf of Lion buoy <bold>(b)</bold> and at the Bay of Biscay buoy <bold>(c)</bold>, for the PMA period. Offsets of
12 h and 60 h have been applied between the wind speed measurements in the Gulf of Lion and the Bay of Biscay
respectively and the PMA concentrations observed at Ersa to account for transport time of the air masses.
The PMA concentrations have been averaged by wind speed bins of 1 m s<inline-formula><mml:math id="M366" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. The error bars represent <inline-formula><mml:math id="M367" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mi mathvariant="italic">σ</mml:mi><mml:mo>/</mml:mo><mml:msqrt><mml:mi>N</mml:mi></mml:msqrt></mml:mrow></mml:math></inline-formula>.
Blue curves represents all the PMA measurements, while green and red curves
represent fresh and aged PMA.</p></caption>
            <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f11.png"/>

          </fig>

      <p>To investigate the origin of PMAs as a function of their ageing, we
distinguished the air masses that contain fresh or aged PMA, using the method
defined in Sect. 3.2.1, for the whole campaign. We observe that the
concentration of aged PMA (Fig. <xref ref-type="fig" rid="Ch1.F10"/>b) is constant and does not
depend on the local wind speed, which suggest that the Ersa site is always
impacted by long-range transport containing aged PMA, even if the
concentration is low (0.6 <inline-formula><mml:math id="M368" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.2 <inline-formula><mml:math id="M369" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M370" 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>). On the contrary, we
observe that fresh PMA concentration measured at Ersa (Fig. <xref ref-type="fig" rid="Ch1.F10"/>b)
is highly dependant on the wind speed, following a fit of the form ln
[PMA] <inline-formula><mml:math id="M371" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> <inline-formula><mml:math id="M372" display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M373" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> WS <inline-formula><mml:math id="M374" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> ln(<inline-formula><mml:math id="M375" display="inline"><mml:mrow><mml:msub><mml:mi>M</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) with a correct correlation (<inline-formula><mml:math id="M376" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.59</mml:mn></mml:mrow></mml:math></inline-formula>).
This result indicates that the highest concentration of PMA measured in Ersa
during the campaign corresponds to fresher aerosols and is dependent on the
local meteorological conditions.</p>
      <p>We then compared the wind speed at the two probable regions of emission, the Gulf
of Lion and the Bay of Biscay, to the concentration of PMA, using FLEXPART
results, for the PMA period (22–26 June). To account for the transport time
of PMA, we added a delay of 12 h, which corresponds to the mean transport
time from the Gulf of Lion to Ersa modelled with FLEXPART for the PMA period,
and 60 h for the Bay of Biscay (Fig. <xref ref-type="fig" rid="Ch1.F11"/>b and c). This work was done for the PMA period from
22 to 26 June. In Fig. <xref ref-type="fig" rid="Ch1.F11"/>a, the correlation between the mass
concentration of PMA and the wind speed at Ersa is good for fresh PMA (<inline-formula><mml:math id="M377" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.71</mml:mn></mml:mrow></mml:math></inline-formula>; Fig. <xref ref-type="fig" rid="Ch1.F11"/>a) as presented in the previous paragraph for the
whole campaign. For the Gulf of Lion (Fig. <xref ref-type="fig" rid="Ch1.F11"/>b), the
correlation is good for aged PMA (red curve, <inline-formula><mml:math id="M378" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.87</mml:mn></mml:mrow></mml:math></inline-formula>) while there is no
correlation following this fit for fresh PMA and wind speed at the Gulf of
Lion. The same analysis was done for the Bay of Biscay (Fig. <xref ref-type="fig" rid="Ch1.F11"/>c) but no correlation was found for fresh, aged PMA or all
the PMA regardless of their ageing.</p>
      <p>According to these results, during the PMA period, the PMA that were measured
in Ersa were a mixture of fresh PMA emitted near the Ersa station and of aged
PMA emitted from the Gulf of Lion. It should be noted that measurements of
PMA have also been made when the air masses were coming from the east, but
the concentrations were lower (<inline-formula><mml:math id="M379" display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 2 <inline-formula><mml:math id="M380" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M381" 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>).</p>
      <p>From these results, the most probable zone that brings PMA to Ersa during
ADRIMED regarding altitude, transport time of air masses and local wind speed
would be the Gulf of Lion and the sea close to Ersa, considering that the
buoy at the Bay of Biscay represents the wind speed of the area. Beyond the
scope of this work, an analysis of the emission and transport of marine
aerosols during this PMA period is ongoing and uses the Meso-NH model.</p>
</sec>
<sec id="Ch1.S3.SS2.SSS3">
  <title>PMA physical properties in comparison with dust and BBP periods</title>
      <p>This PMA period represents the background atmospheric conditions that affect
Ersa most of the time. In this section, after an overview of the ADRIMED
field campaign, the number and volume size
distribution of PMA are investigated, as they are fundamental parameters
which estimate the aerosol radiative effects. A comparison with two sporadic events (dust and BBP), which
influence Ersa principally in spring and summer, is also carried out.</p>
      <p>The total number concentration (CPC <inline-formula><mml:math id="M382" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> OPS) during the campaign observes a mean
value of 1900 <inline-formula><mml:math id="M383" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 920 cm<inline-formula><mml:math id="M384" 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> with several short episodes (few hours) of
high concentrations (<inline-formula><mml:math id="M385" display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> 5000 cm<inline-formula><mml:math id="M386" 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>) at the end of June. Thus, the
background number concentration is higher than what is usually measured at a
pristine marine site (300–600 cm<inline-formula><mml:math id="M387" 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>; <xref ref-type="bibr" rid="bib1.bibx16" id="altparen.70"/>) and denotes
contamination by other sources, principally from continental Europe, as
Ersa is not affected by immediately local sources. In parallel, the number
size distributions measured by the SMPS show that the particles detected
during these short episodes of high concentration have diameters below 50 nm
and probably correspond to new particles during transport over the
Mediterranean sea.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T3" specific-use="star"><caption><p>Characteristics of the fit by  a log-normal distribution (<inline-formula><mml:math id="M388" display="inline"><mml:mi>N</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M389" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M390" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>) for the three periods: dust, PMA and BBP</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="13">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right" colsep="1"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="right" colsep="1"/>
     <oasis:colspec colnum="8" colname="col8" align="right"/>
     <oasis:colspec colnum="9" colname="col9" align="right"/>
     <oasis:colspec colnum="10" colname="col10" align="right" colsep="1"/>
     <oasis:colspec colnum="11" colname="col11" align="right"/>
     <oasis:colspec colnum="12" colname="col12" align="right"/>
     <oasis:colspec colnum="13" colname="col13" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Number concentration</oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math id="M391" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3"><inline-formula><mml:math id="M392" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col4"><inline-formula><mml:math id="M393" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5"><inline-formula><mml:math id="M394" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col6"><inline-formula><mml:math id="M395" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col7"><inline-formula><mml:math id="M396" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col8"><inline-formula><mml:math id="M397" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col9"><inline-formula><mml:math id="M398" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col10"><inline-formula><mml:math id="M399" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col11"><inline-formula><mml:math id="M400" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col12"><inline-formula><mml:math id="M401" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col13"><inline-formula><mml:math id="M402" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">Dust</oasis:entry>  
         <oasis:entry colname="col2">156</oasis:entry>  
         <oasis:entry colname="col3">0.06</oasis:entry>  
         <oasis:entry colname="col4">1.88</oasis:entry>  
         <oasis:entry colname="col5">389</oasis:entry>  
         <oasis:entry colname="col6">0.13</oasis:entry>  
         <oasis:entry colname="col7">1.51</oasis:entry>  
         <oasis:entry colname="col8">0.11</oasis:entry>  
         <oasis:entry colname="col9">1.16</oasis:entry>  
         <oasis:entry colname="col10">1.3</oasis:entry>  
         <oasis:entry colname="col11">0.02</oasis:entry>  
         <oasis:entry colname="col12">3</oasis:entry>  
         <oasis:entry colname="col13">1.47</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PMA</oasis:entry>  
         <oasis:entry colname="col2">1162</oasis:entry>  
         <oasis:entry colname="col3">0.04</oasis:entry>  
         <oasis:entry colname="col4">1.46</oasis:entry>  
         <oasis:entry colname="col5">164</oasis:entry>  
         <oasis:entry colname="col6">0.13</oasis:entry>  
         <oasis:entry colname="col7">1.56</oasis:entry>  
         <oasis:entry colname="col8">0.45</oasis:entry>  
         <oasis:entry colname="col9">1.2</oasis:entry>  
         <oasis:entry colname="col10">1.5</oasis:entry>  
         <oasis:entry colname="col11">0.02</oasis:entry>  
         <oasis:entry colname="col12">5.4</oasis:entry>  
         <oasis:entry colname="col13">1.25</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">BBP</oasis:entry>  
         <oasis:entry colname="col2">0.13</oasis:entry>  
         <oasis:entry colname="col3">0.027</oasis:entry>  
         <oasis:entry colname="col4">0.9</oasis:entry>  
         <oasis:entry colname="col5">582</oasis:entry>  
         <oasis:entry colname="col6">0.08</oasis:entry>  
         <oasis:entry colname="col7">1.79</oasis:entry>  
         <oasis:entry colname="col8">170</oasis:entry>  
         <oasis:entry colname="col9">0.22</oasis:entry>  
         <oasis:entry colname="col10">1.35</oasis:entry>  
         <oasis:entry colname="col11">0.07</oasis:entry>  
         <oasis:entry colname="col12">1.5</oasis:entry>  
         <oasis:entry colname="col13">1.7</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Volume concentration</oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math id="M403" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3"><inline-formula><mml:math id="M404" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col4"><inline-formula><mml:math id="M405" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5"><inline-formula><mml:math id="M406" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col6"><inline-formula><mml:math id="M407" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col7"><inline-formula><mml:math id="M408" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col8"><inline-formula><mml:math id="M409" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col9"><inline-formula><mml:math id="M410" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col10"><inline-formula><mml:math id="M411" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col11"><inline-formula><mml:math id="M412" display="inline"><mml:mrow><mml:msub><mml:mi>V</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col12"><inline-formula><mml:math id="M413" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col13"><inline-formula><mml:math id="M414" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Dust</oasis:entry>  
         <oasis:entry colname="col2">0.5</oasis:entry>  
         <oasis:entry colname="col3">0.18</oasis:entry>  
         <oasis:entry colname="col4">1.46</oasis:entry>  
         <oasis:entry colname="col5">0.64</oasis:entry>  
         <oasis:entry colname="col6">0.26</oasis:entry>  
         <oasis:entry colname="col7">1.43</oasis:entry>  
         <oasis:entry colname="col8">0.43</oasis:entry>  
         <oasis:entry colname="col9">2.36</oasis:entry>  
         <oasis:entry colname="col10">1.62</oasis:entry>  
         <oasis:entry colname="col11"/>  
         <oasis:entry colname="col12"/>  
         <oasis:entry colname="col13"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PMA</oasis:entry>  
         <oasis:entry colname="col2">0.09</oasis:entry>  
         <oasis:entry colname="col3">0.07</oasis:entry>  
         <oasis:entry colname="col4">1.47</oasis:entry>  
         <oasis:entry colname="col5">0.44</oasis:entry>  
         <oasis:entry colname="col6">0.24</oasis:entry>  
         <oasis:entry colname="col7">1.54</oasis:entry>  
         <oasis:entry colname="col8">1.02</oasis:entry>  
         <oasis:entry colname="col9">1.64</oasis:entry>  
         <oasis:entry colname="col10">1.71</oasis:entry>  
         <oasis:entry colname="col11">0.18</oasis:entry>  
         <oasis:entry colname="col12">6.66</oasis:entry>  
         <oasis:entry colname="col13">1.34</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">BBP</oasis:entry>  
         <oasis:entry colname="col2">0.77</oasis:entry>  
         <oasis:entry colname="col3">0.2</oasis:entry>  
         <oasis:entry colname="col4">1.54</oasis:entry>  
         <oasis:entry colname="col5">1.34</oasis:entry>  
         <oasis:entry colname="col6">0.32</oasis:entry>  
         <oasis:entry colname="col7">1.33</oasis:entry>  
         <oasis:entry colname="col8">0.31</oasis:entry>  
         <oasis:entry colname="col9">2.24</oasis:entry>  
         <oasis:entry colname="col10">1.55</oasis:entry>  
         <oasis:entry colname="col11">0.2</oasis:entry>  
         <oasis:entry colname="col12">6.13</oasis:entry>  
         <oasis:entry colname="col13">1.36</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <?xmltex \floatpos{t}?><fig id="Ch1.F12" specific-use="star"><caption><p>Number <bold>(a)</bold> and volume <bold>(b)</bold> size distribution averaged by periods of dust, PMA, and BBP using the
SMPS and OPS instruments. The dry diameters range 10 nm to 10 <inline-formula><mml:math id="M415" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. The first and last days of each
period were removed to capture the main feature and the maximum amplitude of the event.</p></caption>
            <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f12.png"/>

          </fig>

      <p>During this field campaign, the fine and accumulation modes
(10 nm <inline-formula><mml:math id="M416" display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> Dp <inline-formula><mml:math id="M417" display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 600 nm) were dominant in number. Furthermore, the concentration of these two
modes rises at the beginning of July, particularly the accumulation mode,
following the scheme already mentioned in the previous section for PM<inline-formula><mml:math id="M418" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula>
particles. Hence, the ratio of the number concentration from 4 to 13 July over
the number concentration from 6 June to 3 July is greater than 2 for particle
diameters greater than 0.24 and 0.52 <inline-formula><mml:math id="M419" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. This ratio reaches its
highest value for particles with diameters of 0.4 <inline-formula><mml:math id="M420" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m.</p>
      <p>Before conducting comparisons on the physical properties of sea salt, the PMA period
was divided into several shorter periods according to their ageing (see Sect. 3.2.1), that will be called “ageing periods”. In addition, we chose a
supplementary period (1–4 July) corresponding to low PMA concentration when
it does not exceed the background concentration (0.76 <inline-formula><mml:math id="M421" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M422" 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
number and volume size distribution were averaged over the ageing periods and
fitted under the assumption that the distribution is a sum of log-normal modes
to investigate whether the ageing of PMA could be characterised by their size
distributions. Three to six modes were necessary to fit the observed dry size
distributions.</p>
      <p>For the number size distribution, a large variety of Aitken and accumulation
mode can be derived when comparing the different periods. They show a large
variety of diameters and concentration whether they contain low or high PMA
concentration, aged or fresh. However, a coarse mode (modal diameter of 1.2 <inline-formula><mml:math id="M423" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) appears for all the size distributions containing PMA, for both aged
and fresh aerosols. This mode does not exist when the concentration of PMA is
within the background. The concentration of this mode seems to be higher for
fresh than aged PMA which is probably due to dry deposition during transport.
As we did not find any significant difference between the size distributions
of aged and fresh PMA, they are merged for the sequence of the analysis as
PMA size distribution over the PMA period.</p>
      <p>The number and volume size
distribution have been averaged for each periods: dust, PMA and BBP (Fig. <xref ref-type="fig" rid="Ch1.F12"/>). We chose to average the most intense part of each period to
extract the representative properties of each aerosol type. Thus, although
the dust event starts on 16 and ends on 20 June, we analysed the size distribution
obtained from 17:00 to 19 June at 00:00 UTC. Likewise, the study of the size
distribution for PMA and BBP aerosols are from 23 June at 00:00 to 25 June at 00:00 UTC and from 9 July at 00:00 to 11 July 0:00 UTC
respectively. The results are
summarised in Table <xref ref-type="table" rid="Ch1.T3"/>. The highest number concentration for PMA
period was for particles of modal diameter of 40 nm, followed by a mode at
130 nm and a third mode at 1.2 <inline-formula><mml:math id="M424" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. We find a good agreement of modal
diameters with the size distribution measured by <xref ref-type="bibr" rid="bib1.bibx66" id="text.71"/>
in the parameterisation of the emission of PMA from the Atlantic Ocean.
Furthermore, our results agree with measurements taken in the
Mediterranean Sea by <xref ref-type="bibr" rid="bib1.bibx76" id="text.72"/>. We observed a high number
concentration of fine particles during the PMA period, which is consistent with
measurements reported in Fig. <xref ref-type="fig" rid="Ch1.F12"/> a. The modal diameter of these fine
particles is situated at 40 nm. This mode was also measured by
<xref ref-type="bibr" rid="bib1.bibx76" id="text.73"/> at <inline-formula><mml:math id="M425" display="inline"><mml:mrow><mml:mi>d</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">37.5</mml:mn></mml:mrow></mml:math></inline-formula> nm <inline-formula><mml:math id="M426" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.4 during PMA flux
measurements from Mediterranean waters. The second mode has a modal diameter
of 130 nm, which is somewhat higher than the 90 nm mode found by
<xref ref-type="bibr" rid="bib1.bibx76" id="text.74"/>, which is related to the presence of aged
particles during our study.</p>
      <p>We find important distinctions between the three different periods
reported in Fig. <xref ref-type="fig" rid="Ch1.F12"/>a. As expected, during the dust event, the number
size distribution is higher for the largest particles (3 to 10 <inline-formula><mml:math id="M427" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m size
range). During the BBP period, the dominant mode of the number size distribution
is located around 200 nm and the number concentration of particles greater
than 500 nm is found to be low (65 <inline-formula><mml:math id="M428" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 14 cm<inline-formula><mml:math id="M429" 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>). This result is
consistent with the typical number concentration of biomass burning aerosols
that peaks in the size range of 100–200 nm <xref ref-type="bibr" rid="bib1.bibx38 bib1.bibx72 bib1.bibx3" id="paren.75"/>. These hydrophilic aerosols are
subject to increases in size when they age during transport
<xref ref-type="bibr" rid="bib1.bibx2" id="paren.76"/>, which is consistent with our observations of a mode
centred at 200 nm as they were transported for 3–4 days before reaching Ersa.</p>
      <p>Looking at the volume size distribution is a way to distinguish the particles
that have the greatest impact on mass concentration, i.e. the coarser
particles. On average, during the ADRIMED period the mean total volume
concentration (CPC <inline-formula><mml:math id="M430" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> OPS) is 40 <inline-formula><mml:math id="M431" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 16 <inline-formula><mml:math id="M432" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m<inline-formula><mml:math id="M433" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:math></inline-formula> cm<inline-formula><mml:math id="M434" 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 the
volume concentration of smallest particles (<inline-formula><mml:math id="M435" display="inline"><mml:mrow><mml:mi>d</mml:mi><mml:mo>&lt;</mml:mo></mml:mrow></mml:math></inline-formula> 500 nm) is 22 <inline-formula><mml:math id="M436" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 11 <inline-formula><mml:math id="M437" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m<inline-formula><mml:math id="M438" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:math></inline-formula> cm<inline-formula><mml:math id="M439" 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>, while that of the
coarser particles (<inline-formula><mml:math id="M440" display="inline"><mml:mrow><mml:mi>d</mml:mi><mml:mo>&gt;</mml:mo></mml:mrow></mml:math></inline-formula> 500 nm) is 16 <inline-formula><mml:math id="M441" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 9 <inline-formula><mml:math id="M442" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m<inline-formula><mml:math id="M443" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:math></inline-formula> cm<inline-formula><mml:math id="M444" 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>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F13"><caption><p>AERONET volume size distributions averaged for the three periods.</p></caption>
            <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f13.png"/>

          </fig>

      <p>The volume size distribution shows different patterns for the dust, PMA and
BBP periods. We distinguish a coarser mode between 20 and 27 June, including the PMA
period, with a modal diameter of 1.6 <inline-formula><mml:math id="M445" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Marine aerosols with diameters
greater than 1 <inline-formula><mml:math id="M446" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m are largely inorganic sea salt
<xref ref-type="bibr" rid="bib1.bibx64" id="paren.77"/>. A coarse mode is also observed around 19 June
(dust period) with diameters between 5 and 7 <inline-formula><mml:math id="M447" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, which probably corresponds to
mineral dust particles in accordance with the volume size distributions
measured on board the ATR-42 aircraft <xref ref-type="bibr" rid="bib1.bibx18" id="paren.78"/>. Figure <xref ref-type="fig" rid="Ch1.F12"/>b shows two dominant modes during the dust period: one at a dry
diameter of 0.18 <inline-formula><mml:math id="M448" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and the second one around 2.4 <inline-formula><mml:math id="M449" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Finally, the
BBP event is found to be dominated by a mode at 320 nm, and the volume
concentration of the coarse mode is here very low.</p>
      <p>We have also compared the results of the in situ surface volume size
distributions with AERONET/PHOTONS retrievals (Fig. <xref ref-type="fig" rid="Ch1.F13"/>).
AERONET data are compared with the in situ measurements, as they
are derived from an algorithm, averaged over a few days and have a
limited number of measurements (seven available for the PMA period). Concerning
dust and PMA periods, the coarse modes measured by OPS and SMPS are
consistent with the atmospheric column volume size distribution and
contribute to the largest fraction of aerosol mass, even though a fine mode
is also detected during dust periods. During the BBP period, both observations
(in situ and AERONET) clearly indicate volume size distributions that are largely
dominated by the fine mode. The difference of size distribution between the
three periods is higher for AERONET data than for the in situ data. For the
dust period, the reason is that the main part of the dust plume was situated
at an altitude of 3 to 6 km. For the PMA period, the hygroscopic growth of marine
aerosols can explain a shift in the diameter modes. There also might be a
loss of supermicron mode particles before they reach the OPS, which has an
impact on the PMA and dust periods.</p>
      <p>These three periods are characterised by different volume size distributions
(in situ measurements), as summarised in Table <xref ref-type="table" rid="Ch1.T3"/>. The dust and PMA
periods are characterised by coarser particles, with a modal diameter of 2.4
and 1.6 <inline-formula><mml:math id="M450" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m respectively, while the BBP period is characterised by
particles in the accumulation mode with modal diameter of 320 nm.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T4" specific-use="star"><caption><p>Summary of the optical properties (mean and standard deviation) estimated for the three
different aerosols regimes: AOD, AE, SSA, scattering coefficient (in Mm<inline-formula><mml:math id="M451" 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 instantaneous TOA and BOA radiative effect (in W m<inline-formula><mml:math id="M452" 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></caption><oasis:table frame="topbot"><oasis:tgroup cols="7">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="right"/>
     <oasis:thead>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">AOD</oasis:entry>  
         <oasis:entry colname="col3">AE</oasis:entry>  
         <oasis:entry colname="col4">SSA</oasis:entry>  
         <oasis:entry colname="col5">Scattering coefficient</oasis:entry>  
         <oasis:entry colname="col6">TOA</oasis:entry>  
         <oasis:entry colname="col7">BOA</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">500 nm</oasis:entry>  
         <oasis:entry colname="col3">440–870 nm</oasis:entry>  
         <oasis:entry colname="col4">440 nm</oasis:entry>  
         <oasis:entry colname="col5">550 nm</oasis:entry>  
         <oasis:entry colname="col6"/>  
         <oasis:entry colname="col7"/>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">Dust</oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math id="M453" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.16</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.08</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3"><inline-formula><mml:math id="M454" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.4</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">0.3</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col4"><inline-formula><mml:math id="M455" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.97</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.03</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5"><inline-formula><mml:math id="M456" display="inline"><mml:mrow><mml:mn mathvariant="normal">28</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col6"><inline-formula><mml:math id="M457" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">14</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">6</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col7"><inline-formula><mml:math id="M458" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">21</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PMA</oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math id="M459" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.11</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">0.08</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3"><inline-formula><mml:math id="M460" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.3</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.4</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col4"><inline-formula><mml:math id="M461" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.98</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5"><inline-formula><mml:math id="M462" display="inline"><mml:mrow><mml:mn mathvariant="normal">28</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col6"><inline-formula><mml:math id="M463" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">8</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col7"><inline-formula><mml:math id="M464" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">11</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">BBP</oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math id="M465" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.23</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">0.07</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3"><inline-formula><mml:math id="M466" display="inline"><mml:mrow><mml:mn mathvariant="normal">2.1</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.2</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col4"><inline-formula><mml:math id="M467" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.98</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.03</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5"><inline-formula><mml:math id="M468" display="inline"><mml:mrow><mml:mn mathvariant="normal">54</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">18</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col6"><inline-formula><mml:math id="M469" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">15</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col7"><inline-formula><mml:math id="M470" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">23</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">6</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">ADRIMED</oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math id="M471" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.17</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.1</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3"><inline-formula><mml:math id="M472" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.7</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">0.5</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col4"><inline-formula><mml:math id="M473" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.98</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">0.03</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5"><inline-formula><mml:math id="M474" display="inline"><mml:mrow><mml:mn mathvariant="normal">37</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">20</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col6"><inline-formula><mml:math id="M475" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">12</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col7"><inline-formula><mml:math id="M476" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">17</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">8</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

</sec>
<sec id="Ch1.S3.SS2.SSS4">
  <title>PMA optical properties and local shortwave direct radiative effect in comparison with dust and BBP periods</title>
      <p>In addition to chemical and size distribution aerosol properties, we also
determined optical properties, providing AOD at the measuring site, as well as
the SSA and AE obtained for the whole atmospheric column from AERONET/PHOTONS
observations <xref ref-type="bibr" rid="bib1.bibx24" id="paren.79"/> and their spectral dependences in the
solar spectral region. These results are summarised in Table <xref ref-type="table" rid="Ch1.T4"/>. As
in the previous part, a comparison with dust and BBP period was also
realised.</p>
      <p>First, the AOD retrievals provide information about the loading of aerosols
within the atmospheric column. During the ChArMEx-ADRIMED campaign, AOD (at
500 nm) was found to be moderate, with an average of 0.15 <inline-formula><mml:math id="M477" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08 (Fig. <xref ref-type="fig" rid="Ch1.F14"/>a). Such values are consistent with the site location and
aerosol concentration (see Sect. 3.3.1), Ersa not being impacted by local
pollution or high anthropogenic sources. In that sense, the AOD background is
low, typical of a rural site. However, from the beginning of July to the end
of the campaign, the AOD increases to values up to 0.6 with a higher
wavelength dependency.</p>
      <p>AOD is lowest during the PMA event (22–26 June), with a mean value of 0.11 <inline-formula><mml:math id="M478" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08 at 500 nm, close to those reported over the Mediterranean Basin
<xref ref-type="bibr" rid="bib1.bibx84 bib1.bibx67 bib1.bibx29" id="paren.80"/>. <xref ref-type="bibr" rid="bib1.bibx83" id="text.81"/> found
that for clean oceanic conditions, AOD was below 0.1 (at 550 nm) and
<xref ref-type="bibr" rid="bib1.bibx67" id="text.82"/> found an average value of 0.11 for the same marine
conditions. In the Mediterranean sea in particular, <xref ref-type="bibr" rid="bib1.bibx29" id="text.83"/>
reported a value of 0.15 in Crete in the background corresponding to
marine aerosols and <xref ref-type="bibr" rid="bib1.bibx57" id="text.84"/> found a mean AOD over the eastern
Mediterranean for marine aerosols (June–August 2010) of 0.06 <inline-formula><mml:math id="M479" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01.
Furthermore, it should be noted that AOD is not very sensitive to the
wavelengths during these 5 days due to the presence of coarse particles.</p>
      <p>AOD is higher during the dust event, reaching 0.3 (at 500 nm; Fig. <xref ref-type="fig" rid="Ch1.F14"/>), corresponding to a relatively low value for a dust
outbreak occurring over the Mediterranean Basin <xref ref-type="bibr" rid="bib1.bibx53" id="paren.85"/>. AOD can
reach values above one (<xref ref-type="bibr" rid="bib1.bibx37" id="altparen.86"/>, over the western
Mediterranean) and even up to two (<xref ref-type="bibr" rid="bib1.bibx21" id="altparen.87"/> over Lampedusa).
As observed during the PMA period, AOD is not sensitive to wavelengths during the
dust event, denoting the presence of coarse particles. AOD showed a very
different pattern during the last part of the campaign, reaching higher
values and showing a strong dependence to the wavelengths. AOD thus exceeds
0.4 in the middle of July and is higher for shorter wavelengths. It denotes a
significant contribution of small particles to the solar extinction, in
accordance with the SMPS and TEOM PM<inline-formula><mml:math id="M480" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> observations previously presented and
during the BBP period. The AOD values are much higher for these two periods
than for the PMA period.</p>
      <p>For the PMA episode, AE varied between 0.4 and 2, with a mean value of 1.3, which
is below the mean value of the ADRIMED campaign (1.8; Fig. <xref ref-type="fig" rid="Ch1.F14"/>b). AE also decreased to 1.15 for 24 June, when PMA concentration is
highest. Such a value is characteristic of clean ocean regions as reported by
<xref ref-type="bibr" rid="bib1.bibx84" id="text.88"/>, who found values between 0.3 and 0.7. In addition,
<xref ref-type="bibr" rid="bib1.bibx67" id="text.89"/> and <xref ref-type="bibr" rid="bib1.bibx29" id="text.90"/> reported AE between 0.7
and 1 for background marine atmosphere over the central and eastern
Mediterranean. The AE measured at the Ersa station during the PMA event is not as
low as these referenced values and could indicate a possible mixing between
sea salt and other aerosols, as the western Mediterranean is under the
permanent influence of continental sources. This point is also consistent
with the observed number size distribution, which showed that the number
concentration of fine particles was high during the PMA event, indicating
pollution particles from the European continent.</p>
      <p>A high variability was also found during dust periods. Indeed, AE fluctuated
between 1 and 2. These are not typical values observed for desert dust particles,
which generally tend toward values less than one, denoting a majority of
coarse particles <xref ref-type="bibr" rid="bib1.bibx23" id="paren.91"/>. In that sense, the higher
values observed at Ersa could be due to the possible mixing of particles in
the atmosphere during these days, by the weak intensity of the dust outbreak
observed during ADRIMED or by the possible deposition of the coarser dust
particles during transport. Finally, and during the BBP period, AE was found to be
mostly above two. Its pattern follows a clear diurnal variation, with a
maximum around 12:00 UTC and a minimum in the beginning and in the end of the
day. AE observed during this period is stable for almost a week, from 4 to 10
July. The largest difference noted for AE between dust, PMA and BBP periods
is in their internal variability. For the first two periods, a mixing and
high variability is found while for the last period, AE is constant for more
than 5 days, showing that the atmosphere is mostly under the influence of the
same aerosol type.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F14" specific-use="star"><caption><p>Time series of <bold>(a)</bold> aerosol optical depth (AOD) at three
wavelengths (440, 500 and 870 nm) measured by the radiometer from the
AERONET network situated at the Semaphore during the ADRIMED campaign,
<bold>(b)</bold> Ångström exponent calculated from AERONET data, during
the ADRIMED campaign, using the extinction measurements at 440 and 870 nm,
<bold>(c)</bold> Scattering coefficient at three wavelengths: 450 nm (blue),
550 nm (green) and 700 nm (red) measured by the nephelometer situated at
Ersa.</p></caption>
            <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f14.png"/>

          </fig>

      <p>Overall, SSA observed during the campaign remained relatively high, with
values above 0.90 for most of the period, associated with a spectral dependence
less than 0.05 (from 440 to 870 nm). In that sense, the presence of absorbing
particles is shown to be sporadic and lasted no more than a few hours. During
the PMA period, SSA was found close to unity (mean of 0.98 <inline-formula><mml:math id="M481" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02; not shown
here), indicating significant scattering optical properties, consistent with
marine aerosols optical properties in the solar range <xref ref-type="bibr" rid="bib1.bibx49" id="paren.92"/>.
During the dust period 16–20 June, SSA decreased to values between 0.90 and 0.95
(at 440 nm), indicating moderate absorbing properties, which are
characteristics of desert dust over the Mediterranean Basin
<xref ref-type="bibr" rid="bib1.bibx52" id="paren.93"/>. Finally, during the BBP period, we observed a
higher wavelength dependency, with SSA values oscillating between 0.90 and
1.0 (at 440 nm).</p>
      <p>In addition to the atmospheric column information, over the entire period of
the campaign, nephelometer measurements reveal that the scattering due to
particles was relatively low (mean of 37 Mm<inline-formula><mml:math id="M482" 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> <inline-formula><mml:math id="M483" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 20, at 550 nm) and
not sensitive to wavelength during June, particularly during dust and PMA
periods (Fig. <xref ref-type="fig" rid="Ch1.F14"/>c). This is in contrast to July, when higher
scattering coefficients (mean of 48 Mm<inline-formula><mml:math id="M484" 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> <inline-formula><mml:math id="M485" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 24) associated with
higher AE (AE July mean of 2.1 <inline-formula><mml:math id="M486" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.2, AE June mean of 1.6 <inline-formula><mml:math id="M487" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.5) are
observed.</p>
      <p>During dust and PMA period, the scattering coefficient remains low (mean of
28 <inline-formula><mml:math id="M488" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 11 and 28 <inline-formula><mml:math id="M489" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 11 Mm<inline-formula><mml:math id="M490" 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> respectively). The PMA period is
characterised by a relatively weak wavelength dependency (Fig. <xref ref-type="fig" rid="Ch1.F14"/>c). While the mixing of dust with fine particles,
previously shown by the AERONET volume size distribution, is shown here by a
relatively high wavelength dependency (mean of 20 <inline-formula><mml:math id="M491" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 9 Mm<inline-formula><mml:math id="M492" 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>). On the
contrary, during the BBP period, the wavelength dependency is highest (mean
of 49 <inline-formula><mml:math id="M493" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 15 Mm<inline-formula><mml:math id="M494" 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 450 and 700 nm), and the scattering
coefficient reaches its highest values (up to 137 Mm<inline-formula><mml:math id="M495" 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>). This clearly
indicates that aerosols are smaller in size during this period, which is
consistent with AERONET/PHOTONS data and PM<inline-formula><mml:math id="M496" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:math></inline-formula> concentrations obtained at
Ersa station.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F15" specific-use="star"><caption><p>Aerosol radiative effect at <bold>(a)</bold> the top of the atmosphere (TOA) and <bold>(b)</bold> the bottom of the atmosphere (BOA)
represented as a function of the aerosol optical thickness (AOT) for each of the major periods, retrieved from AERONET.</p></caption>
            <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://acp.copernicus.org/articles/17/7891/2017/acp-17-7891-2017-f15.png"/>

          </fig>

      <p>The optical characteristics (AOD, SSA and AE) of the air masses during the
PMA event are found to be consistent with the literature <xref ref-type="bibr" rid="bib1.bibx84 bib1.bibx67" id="paren.94"/>, even though a mixing with continental fine particles was also
detected.</p>
      <p>In parallel to optical properties observations, the local 1-D (clear-sky)
direct radiative effect (DRE) in the shortwave (SW) spectral region has been
estimated using AERONET/PHOTONS retrievals <xref ref-type="bibr" rid="bib1.bibx32" id="paren.95"/> for
each identified period. DRE is calculated here at two different atmospheric
levels: at the surface (bottom of the atmosphere, BOA) and at the top of
the atmosphere (TOA). Figure <xref ref-type="fig" rid="Ch1.F15"/>b indicates the SW DRE at BOA for
different AOD and different solar angles observed during the experiment. The
estimated values show significant variability with instantaneous DRE
between <inline-formula><mml:math id="M497" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5 and <inline-formula><mml:math id="M498" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>40 W m<inline-formula><mml:math id="M499" 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>, depending on the aerosol regimes.
Figure <xref ref-type="fig" rid="Ch1.F15"/>a and b) indicates that PMA period is characterised by
moderate TOA DRE (mean of <inline-formula><mml:math id="M500" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>8 <inline-formula><mml:math id="M501" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3 W m<inline-formula><mml:math id="M502" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) and BOA DRE (mean of <inline-formula><mml:math id="M503" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>11 <inline-formula><mml:math id="M504" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4 W m<inline-formula><mml:math id="M505" 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>). Such estimates at Ersa station are found to be
consistent with direct SW effects of sea salt documented by
<xref ref-type="bibr" rid="bib1.bibx51" id="text.96"/>,
who used the COSMO-ART model over the Mediterranean Basin and reported a SW DRE
from <inline-formula><mml:math id="M506" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>5 to <inline-formula><mml:math id="M507" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>10 W m<inline-formula><mml:math id="M508" 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> at the surface and an AOD between 0.1
and 0.2 (at 550 nm).</p>
      <p>The highest values of BOA DRE correspond to the highest AOD observed during dust
event. For this specific event, values with peak maxima of -43 W m<inline-formula><mml:math id="M509" 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>
are in the same range of magnitude of values reported for mineral dust
aerosols over the Mediterranean Basin by <xref ref-type="bibr" rid="bib1.bibx19" id="text.97"/>. Intermediate
BOA DRE are calculated under polluted and biomass burning influence (from
5–12 July), and range from <inline-formula><mml:math id="M510" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>13 to <inline-formula><mml:math id="M511" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>38 W m<inline-formula><mml:math id="M512" 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>. Such values are classically
derived over the western Mediterranean for polluted particles
<xref ref-type="bibr" rid="bib1.bibx74" id="paren.98"/>.</p>
      <p>In addition, the calculated SW DRE at TOA is reported in Fig. <xref ref-type="fig" rid="Ch1.F15"/>a,
showing negative effects in all conditions due to the moderate absorbing
ability of aerosols associated with a low surface albedo at Ersa (Nicolas et
al., 2017) and leading to cooling at TOA. It should be noted that the DRE of
aerosols in the longwave (LW) spectral range, which can counterbalance a
part of the SW cooling at TOA, is not estimated here. Contrary to the LW DRE
of mineral dust exerted near dust sources, this effect is generally lower
than SW DRE during the transport of mineral dust over the Mediterranean Basin
<xref ref-type="bibr" rid="bib1.bibx60" id="paren.99"/>. In the same way as at the surface, Fig. <xref ref-type="fig" rid="Ch1.F15"/>b indicates that higher TOA DRE occur during the mineral dust event, with
values as large as <inline-formula><mml:math id="M513" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>20 to <inline-formula><mml:math id="M514" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>25 W m<inline-formula><mml:math id="M515" 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>, but due to the spread of the values
during the episode, the mean value of TOA DRE is in the same range as for
BBP period. Finally, we report logically intermediate TOA DRE (mean of <inline-formula><mml:math id="M516" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>15 <inline-formula><mml:math id="M517" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4 W m<inline-formula><mml:math id="M518" 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>) between 5 and 12 July, when Ersa station is affected by
pollution and smoke aerosols.</p>
      <p>To conclude, PMA SW DRE at TOA and BOA is 2 or 3 times lower than what we
encounter during events like dust outbreaks and biomass burning, which occur
principally in spring and summer. However, the influence of marine aerosols
is permanent, depending particularly on wind speed.</p>
</sec>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <title>Conclusion</title>
      <p>The ChArMEx-ADRIMED campaign that took place in summer 2013 in the western
and central Mediterranean Basin has served to characterise the aerosol
optical, physical and chemical properties, to quantify their direct radiative
effect and study their implications on the regional climate
<xref ref-type="bibr" rid="bib1.bibx53" id="paren.100"/>. One of the ground-based instrumented sites was based in
Ersa, Cap Corse and allowed the study of different aerosol types,
particularly the properties and relative impacts of PMA compared to other
aerosol types present in the western Mediterranean Basin.</p>
      <p>Using FLEXPART back-trajectory simulations and in situ optical, physical and
chemical measurements, we show that Ersa was impacted by air masses coming
from different source regions and bringing different aerosol types. Three
main periods have been identified to characterise the relative impacts of
the major aerosol types and, in particular, a period (22–26 June) when the
Ersa site is mainly affected by PMA. During this period, the Ersa station was
influenced by a westerly wind bringing air masses from the Gulf of Lion, the
Mediterranean coasts of France and Spain and the Bay of Biscay. During this
specific event, the concentration of PMA was relatively high, reaching 6.5 <inline-formula><mml:math id="M519" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math id="M520" 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>, which represents 40 % of the total PM<inline-formula><mml:math id="M521" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msub></mml:math></inline-formula> mass
concentration. Here, an original data set, obtained from ATOFMS and PILS-IC
instruments has been used to study the ageing of PMA. By comparing the two
instruments, we found that the majority of the time PMA had already undergone
chemical reactions and so were not freshly emitted near Cap Corse, but
rather advected from long-range transport. In particular, during the PMA
period, based on FLEXPART simulations and local wind speed measurements, we
distinguished the origin of fresh and aged PMA composing the mixing of PMA
observed in the Ersa station. We found that fresh PMAs were emitted near the
station under high wind speed conditions while aged PMAs were most probably
originating from the Gulf of Lion (Mediterranean) and not from the Bay of
Biscay (North Atlantic Ocean).</p>
      <p>These two original instruments display similar results regarding PMA ageing,
and detect different short periods (of few hours duration) of mostly aged or
mostly fresh PMA dominance that we used for our analysis.</p>
      <p>No significant distinction was found between the number size distribution of
fresh and aged supermicron PMA, and so the size distribution was fitted
regardless of the ageing of these aerosols. The log-normal modes (four modes with
diameters of 0.04, 0.13, 1.2 and 5.4 <inline-formula><mml:math id="M522" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) found for these PMA were in
agreement with previous measurement made by <xref ref-type="bibr" rid="bib1.bibx66" id="text.101"/> and
<xref ref-type="bibr" rid="bib1.bibx76" id="text.102"/>. The PMA episode was also influenced by fine
particles, denoted by the high number concentration of fine particle and by
an Ångström exponent varying between 0.4 and 2. In parallel, low AOD (mean of
0.11 at 500 nm) and SSA (at 440 nm) close to unity also measured at Ersa are
typical of the PMA influence. The SW DRF showed the lowest values at the
surface compared to other aerosol regimes with a mean of <inline-formula><mml:math id="M523" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>11 <inline-formula><mml:math id="M524" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4 W m<inline-formula><mml:math id="M525" 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>. At the top of the atmosphere (TOA), the lowest values were also
observed during the PMA event (mean of <inline-formula><mml:math id="M526" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>8 <inline-formula><mml:math id="M527" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3 W m<inline-formula><mml:math id="M528" 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>
      <p>The aerosol properties obtained during this PMA event were compared to two
other periods encountered during the field campaign (dust and BBP). The first
period corresponds to a dust outbreak of moderate intensity (16–20 June;
dust), and the last period (5–12 July) is characterised by biomass burning
that originated in Ukraine and mixed with pollution in southern Europe (BBP). In
terms of physical and chemical properties, our results display large
variability in the number and volume size distribution as well as mass
concentrations between the different events. The volume size distribution
analyses reveal that the BBP event is dominated by a fine mode of particles
with a modal diameter of 320 nm, while the PMA period is dominated by a
coarse mode with a modal diameter of 1.64 <inline-formula><mml:math id="M529" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Finally, dust aerosols
observed at Ersa are characterised by a modal diameter of 2.4 <inline-formula><mml:math id="M530" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, which
is found to be consistent with aircraft in situ observations within dust
plumes in the free troposphere during the airborne portion of the ChArMEx-ADRIMED
experiment <?xmltex \hack{\mbox\bgroup}?><xref ref-type="bibr" rid="bib1.bibx18" id="paren.103"/><?xmltex \hack{\egroup}?>.</p>
      <p>Concerning the optical properties, our results indicate that the dust event
is characterised by a moderate AOD with a mean of 0.16 <inline-formula><mml:math id="M531" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08 and highest
values reaching 0.30 (at 500 nm) associated with a mean AE of 1.4 (calculated
between 440 and 870 nm). SSA during the dust episode (0.97 at 440 nm) is
found to be high, revealing mostly scattering dust aerosols in this case.</p>
      <p>The most intense optical signature clearly occurs at the end of the campaign
during the BBP episode. For this specific period, a significant scattering
coefficient estimated at the surface (mean of 54 Mm<inline-formula><mml:math id="M532" 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 550 nm,
together with moderate AOD (0.23 <inline-formula><mml:math id="M533" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.07 at 500 nm) and elevated spectral
dependence are observed.</p>
      <p>In terms of SW DRF, our results showed the highest (lowest) contribution to
surface effects during the dust (PMA) event with <inline-formula><mml:math id="M534" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>21 <inline-formula><mml:math id="M535" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 11 W m<inline-formula><mml:math id="M536" 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> (<inline-formula><mml:math id="M537" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>11 <inline-formula><mml:math id="M538" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4 W m<inline-formula><mml:math id="M539" 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 intermediate values (<inline-formula><mml:math id="M540" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>23 <inline-formula><mml:math id="M541" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 6 W m<inline-formula><mml:math id="M542" 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>)
observed during the BBP episode. All derived SW DRF at the surface for the
three aerosol types are similar to previous studies in the western
Mediterranean Basin. Similar results are obtained for the top of the
atmosphere (TOA) effect, with the highest values occurring during the dust
outbreak (<inline-formula><mml:math id="M543" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>14 <inline-formula><mml:math id="M544" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 6 W m<inline-formula><mml:math id="M545" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) and BBP period (<inline-formula><mml:math id="M546" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>5 <inline-formula><mml:math id="M547" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4 W m<inline-formula><mml:math id="M548" 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>),
while the lowest values were observed during the PMA event (<inline-formula><mml:math id="M549" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>8 <inline-formula><mml:math id="M550" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3 W m<inline-formula><mml:math id="M551" 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>). Even though the magnitude of PMA DRF is relatively small compared
to dust and BBP DRF, its impact is permanent due to the persistency of PMA in
the marine atmosphere.</p>
</sec>

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

      <p>AERONET/PHOTONS data are available on the website
<uri>https://aeronet.gsfc.nasa.gov/</uri>. The data (FLEXPART back trajectories,
aerosol chemical, physical and optical properties) used in the paper are
part of the ChArMEx-ADRIMED project and are available from the ChArMEx database
by request (<uri>http://mistrals.sedoo.fr/</uri>).</p>
  </notes><notes notes-type="authorcontribution">

      <p>PILS-IC, ACSM, TEOM PM10 and TEOM PM1 data were provided by J. Sciare; ATOFMS data were provided by
J. Arndt and J. Wenger; SMPS, OPS, CPC, Nephelometer and meteorological data were provided by Météo-France.
M. Claeys prepared the manuscript with contributions from all co-authors.</p>
  </notes><notes notes-type="competinginterests">

      <p>The authors declare that they have no conflict of
interest.</p>
  </notes><ack><title>Acknowledgements</title><p>This research was supported by Direction Générale de l'Armement (DGA) and Météo-France.
This research has received funding from the French National Research Agency (ANR) project ADRIMED (contract ANR-11-BS56-0006).
This work is part of the ChArMEx project supported by ADEME, CEA, CNRS-INSU and Météo-France through the
multidisciplinary programme MISTRALS (Mediterranean Integrated Studies aT Regional And Local Scales).
The station at Ersa was partly supported by the CORSiCA project funded by the Collectivité Territoriale
de Corse through the Fonds Européen de Développement Régional of the European Operational Program 2007–2013
and the Contrat de Plan Etat-Région. We acknowledge the AERONET/PHOTONS sun photometer networks and the PI of the
Ersa station and their staff for their work to produce the data set used in this study.
Contributions by Thierry Bourrianne and help from Cyrielle Denjean are gratefully acknowledged.
We gratefully acknowledge the two anonymous reviewers whose comments helped us to improve this manuscript.
Thanks to Laurent Gomez without whom this study would have never taken place.
<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>
Edited by: E. Gerasopoulos<?xmltex \hack{\newline}?>
Reviewed by: two anonymous referees</p></ack><ref-list>
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    <!--<article-title-html>Optical, physical and chemical properties of aerosols transported to a coastal site in the western Mediterranean: a focus on primary marine aerosols</article-title-html>
<abstract-html><p class="p">As part of the ChArMEx-ADRIMED campaign (summer 2013), ground-based
in situ observations were conducted at the Ersa site (northern tip of
Corsica; 533 m a.s.l.) to characterise the optical, physical and chemical
properties of aerosols. During the observation period, a major influence of
primary marine aerosols was detected (22–26 June), with a mass concentration
reaching up to 6.5 µg m<sup>−3</sup> and representing more than 40 % of the
total PM<sub>10</sub> mass concentration. Its relatively low ratio of chloride to
sodium (average of 0.57) indicates a fairly aged sea salt aerosol at
Ersa. In this work, an original data set, obtained from online real-time
instruments (ATOFMS, PILS-IC) has been used to characterise the ageing of
primary marine aerosols (PMAs). During this PMA period, the mixing of fresh and aged PMAs was found
to originate from both local and regional (Gulf of Lion) emissions, according
to local wind measurements and FLEXPART back trajectories. Two different
aerosol regimes have been identified: a dust outbreak (dust) originating from
Algeria/Tunisia, and a pollution period with aerosols originating from
eastern
Europe, which includes anthropogenic and biomass burning sources (BBP). The
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the PMA period with mean values of −11 ± 4 at the surface and
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found for the BBP period to those during the dust period (SW DRF at the surface
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