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

    <article-meta>
      <article-id pub-id-type="doi">10.5194/acp-15-4259-2015</article-id><title-group><article-title><?xmltex \hack{\vspace*{5mm}}?>An overview of regional and local characteristics of aerosols in South Africa using satellite, ground, and modeling data</article-title>
      </title-group><?xmltex \runningtitle{South African aerosol}?><?xmltex \runningauthor{S.~P.~Hersey et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1 aff2">
          <name><surname>Hersey</surname><given-names>S. P.</given-names></name>
          <email>scott.hersey@gmail.com</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2 aff3">
          <name><surname>Garland</surname><given-names>R. M.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1855-8622</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Crosbie</surname><given-names>E.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Shingler</surname><given-names>T.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4 aff5">
          <name><surname>Sorooshian</surname><given-names>A.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-2243-2264</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Piketh</surname><given-names>S.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Burger</surname><given-names>R.</given-names></name>
          
        </contrib>
        <aff id="aff1"><label>1</label><institution>Department of Environmental Sciences and Management, North-West University, Potchefstroom, South Africa</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Now at Franklin W. Olin College of Engineering, Needham, MA, USA</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Council for Scientific and Industrial Research (CSIR), Pretoria, South Africa</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Department of Atmospheric Sciences, University of Arizona, Tucson, AZ, USA</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>Department of Chemical and Environmental Engineering, University of Arizona, Tucson, AZ, USA</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">S. P. Hersey (scott.hersey@gmail.com)</corresp></author-notes><pub-date><day>24</day><month>April</month><year>2015</year></pub-date>
      
      <volume>15</volume>
      <issue>8</issue>
      <fpage>4259</fpage><lpage>4278</lpage>
      <history>
        <date date-type="received"><day>16</day><month>July</month><year>2014</year></date>
           <date date-type="rev-request"><day>25</day><month>September</month><year>2014</year></date>
           <date date-type="rev-recd"><day>25</day><month>March</month><year>2015</year></date>
           <date date-type="accepted"><day>26</day><month>March</month><year>2015</year></date>
      </history>
      <permissions>
<license license-type="open-access">
<license-p>This work is licensed under a Creative Commons Attribution 3.0 Unported License. To view a copy of this license, visit <ext-link ext-link-type="uri" xlink:href="http://creativecommons.org/licenses/by/3.0/">http://creativecommons.org/licenses/by/3.0/</ext-link></license-p>
</license>
</permissions><self-uri xlink:href="https://acp.copernicus.org/articles/.html">This article is available from https://acp.copernicus.org/articles/.html</self-uri>
<self-uri xlink:href="https://acp.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/.pdf</self-uri>


      <abstract>
    <p>We present a comprehensive overview of particulate air quality across the
five major metropolitan areas of South Africa (Cape Town, Bloemfontein,
Johannesburg and Tshwane (Gauteng Province), the Industrial Highveld Air
Quality Priority Area (HVAPA), and Durban), based on a decadal (1 January 2000
to 31 December 2009) aerosol climatology from multiple satellite platforms and
detailed analysis of ground-based data from 19 sites throughout Gauteng
Province. Satellite analysis was based on aerosol optical depth (AOD) from
MODIS Aqua and Terra (550 nm) and MISR (555 nm) platforms, Ångström
Exponent (<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>) from MODIS Aqua (550/865 nm) and Terra (470/660 nm),
ultraviolet aerosol index (UVAI) from TOMS, and results from the
Goddard Ozone Chemistry Aerosol Radiation and Transport (GOCART) model. At
continentally influenced sites, AOD, <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>, and UVAI reach maxima
(0.12–0.20, 1.0–1.8, and 1.0–1.2, respectively) during austral spring
(September–October), coinciding with a period of enhanced dust generation and the
maximum integrated intensity of close-proximity and subtropical fires
identified by MODIS Fire Information for Resource Management System (FIRMS).
Minima in AOD, <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>, and UVAI occur during winter. Results from ground
monitoring indicate that low-income township sites experience by far the
worst particulate air quality in South Africa, with seasonally averaged
PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> concentrations as much as 136 % higher in townships that in
industrial areas.</p>
    <p>We report poor agreement between satellite and ground aerosol measurements,
with maximum surface aerosol concentrations coinciding with minima in AOD,
<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>, and UVAI. This result suggests that remotely sensed data are not an
appropriate surrogate for ground air quality in metropolitan South Africa.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p>The impacts of aerosols on human health, visibility, and climate are
well documented. There are a number of natural sources of dust, sea salt,
sulfate, and organic aerosol, and anthropogenic aerosol primarily derives
from fuel combustion. Combustion aerosol can be directly emitted as soot or
formed in the atmosphere through photochemical reactions that produce
low volatility, secondary sulfate, nitrate, and organic species that either
nucleate to form new aerosol or condense onto existing particles. Exposure to
particulate pollution is typically worst in urban areas, where anthropogenic
emissions are collocated with high population density. The lowest-income
fraction of the population tends to experience the worst air quality because
the least expensive property (or land available for informal settlements) is
often close in proximity to major air pollutant sources like highways, power
generation facilities, or industry. In developing countries, low-income
households are significantly more likely to utilize non-electricity energy
sources such as coal, wood, and paraffin <xref ref-type="bibr" rid="bib1.bibx23 bib1.bibx44" id="paren.1"/>.
Suboptimal burning conditions in domestic settings often result in large
emissions of particulates and particulate precursors, leading to high
concentrations of PM <xref ref-type="bibr" rid="bib1.bibx23 bib1.bibx63 bib1.bibx67" id="paren.2"/>. In South
Africa, the highest concentrations of PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> are measured
in townships and informal settlements during winter, when domestic burning is
most prevalent for heating and cooking, and when emissions are confined in a
shallow boundary layer <xref ref-type="bibr" rid="bib1.bibx23 bib1.bibx63 bib1.bibx67 bib1.bibx65" id="paren.3"/>. A number of reports and peer-reviewed articles have sought to
characterize air quality in low-income areas of South Africa
<xref ref-type="bibr" rid="bib1.bibx18 bib1.bibx19 bib1.bibx20 bib1.bibx23 bib1.bibx44" id="paren.4"><named-content content-type="pre">e.g.,</named-content></xref>, but these studies have typically been limited in geographic scope
and have not characterized the major metropolitan centers where high
densities of South Africans reside.</p>
      <p>There is a wealth of remotely sensed air quality information available from
satellite platforms, and a number of studies have used aerosol optical depth
(AOD or <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">τ</mml:mi></mml:math></inline-formula>) as a proxy for air quality <xref ref-type="bibr" rid="bib1.bibx69 bib1.bibx36 bib1.bibx68 bib1.bibx47 bib1.bibx42 bib1.bibx32 bib1.bibx2 bib1.bibx31 bib1.bibx7 bib1.bibx24 bib1.bibx41 bib1.bibx58 bib1.bibx60 bib1.bibx59 bib1.bibx56 bib1.bibx13" id="paren.5"/>. AOD (aerosol optical depth) typically displays strong
seasonality, with higher AOD observed during periods of peak photochemical
production of secondary aerosol – except in areas where either dust
generation or biomass burning enhances AOD during other seasons. AOD
frequently correlates with ground-based observations of visibility and
particulate concentrations, suggesting that it may be an appropriate
surrogate for particulate matter at the ground in a number of regions.
However, vertical variability in particulate concentrations makes the use of
AOD as a proxy for surface air quality tenuous. For example, concentrated
plumes of particles transported aloft may enhance AOD significantly but not
impact air quality at the ground <xref ref-type="bibr" rid="bib1.bibx6" id="paren.6"><named-content content-type="pre">e.g.,</named-content></xref>. Conversely,
high concentrations of pollutants in a shallow boundary layer with
particle-free air aloft will result in low AOD despite extremely poor air
quality at the ground <xref ref-type="bibr" rid="bib1.bibx13" id="paren.7"><named-content content-type="pre">e.g.,</named-content></xref>. While remotely sensed
AOD may provide an appropriate measure of air quality in some areas, its
general applicability must be evaluated and caution must be exercised when
attempting to use column aerosol data as a surrogate for ground particulate
concentrations.</p>
      <p>Particulates measured at the ground in South Africa are predominately dust,
industrial secondary sulfate, and secondary organics <xref ref-type="bibr" rid="bib1.bibx37 bib1.bibx45 bib1.bibx46 bib1.bibx61" id="paren.8"/>, but significant attention has been
paid to the impact of biomass burning on particulates in the country.
Regional biomass burning in Southern Africa occurs from June to October
<xref ref-type="bibr" rid="bib1.bibx12" id="paren.9"/>, and has been characterized extensively by the Southern
Africa Fire-Atmosphere Research Initiative (SAFARI) studies of 1992 and 2000.
SAFARI-92 and SAFARI-2000 results indicate that transported smoke enhances AOD
significantly in South Africa during August and September
<xref ref-type="bibr" rid="bib1.bibx21 bib1.bibx6 bib1.bibx22 bib1.bibx17 bib1.bibx53 bib1.bibx38 bib1.bibx66 bib1.bibx39 bib1.bibx48 bib1.bibx60 bib1.bibx32" id="paren.10"/>.
The biomass burning emissions that most significantly impact South Africa
originate in neighboring countries – particularly Zimbabwe and Mozambique
<xref ref-type="bibr" rid="bib1.bibx39" id="paren.11"/>. Because these emissions are transported in stratified
layers aloft <xref ref-type="bibr" rid="bib1.bibx6 bib1.bibx9" id="paren.12"/>, they may impact column
aerosol properties such as AOD but not particulate concentrations at the
ground.</p>
      <p>While transported biomass burning has been demonstrated to impact AOD
seasonally, domestic burning – especially for heating and cooking during
winter – is the source associated with the highest particulate concentrations
in South Africa <xref ref-type="bibr" rid="bib1.bibx18 bib1.bibx19 bib1.bibx20" id="paren.13"/>.
Despite work to characterize emission factors and ambient air quality impacts
of domestic burning, studies have been limited in scale to the household or
township level and have never considered the dynamics and impact of domestic
burning emissions across an entire major population center.</p>
      <p>The objective of this work is to characterize aerosol properties in urban
centers in South Africa using satellite and ground based measurements, and to
determine whether remotely sensed data may be used as a proxy for ground air
quality in the region. First we present remotely sensed and modeled column
aerosol data related to total light extinction (AOD), particle size
(Ångström Exponent, <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>), total light absorption (ultraviolet
aerosol index, UVAI), and AOD contribution from individual chemical
components (Goddard Ozone Chemistry Aerosol Radiation and Transport, GOCART).
Satellite data are focused on the five metropolitan and industrial areas of
South Africa with highest population density (Cape Town, Bloemfontein,
Gauteng Province, Industrial Highveld Air Quality Priority Area or HVAPA, and
Durban). We then investigate ground-based measurements of particulate matter
(PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula>) within the satellite study area that comprises the
Johannesburg and Tshwane metropolitan areas (Gauteng Province) in order to
understand seasonal, diurnal and regional trends in particulate
concentrations across the primary environment types common to all major South
African population centers: townships, urban/suburban residential areas, and
industrial areas. We finally explore connections between remotely sensed and
ground data in order to determine whether satellite-derived aerosol
parameters are appropriate surrogates for air quality at the ground in the
South African context. This work expands on results from the SAFARI campaigns
by investigating decadal averages in aerosol column properties during all
seasons and across the country's major metropolitan areas. Further, it offers
a quantitative treatment of particulate air quality characteristic of upper
and lower income residential and industrial areas in the country. These
results are highly relevant to epidemiologists as well as community,
industry, and government stakeholders aiming to understand and improve
particulate air quality for South Africans.</p>
</sec>
<sec id="Ch1.S2">
  <title>Data and methods</title>
      <p>This study utilizes a combination of remotely sensed and ground-based
observations of atmospheric particulates across South Africa. Rather than
define study areas based on large geographical regions that require
significant data averaging <xref ref-type="bibr" rid="bib1.bibx60" id="paren.14"><named-content content-type="pre">e.g.,</named-content></xref>, we focused our
study of remotely sensed data on five smaller study areas that comprise the
five major metropolitan and centers of population density in South Africa
(Cape Town, Bloemfontein, Gauteng Province, Industrial Highveld Air Quality
Priority Area or HVAPA, and Durban; Fig. <xref ref-type="fig" rid="Ch1.F1"/>). We then utilized
data from four networks of ground-based air quality monitoring from the South
African Air Quality Information System (SAAQIS) for one of these study areas
(Gauteng; see Table <xref ref-type="table" rid="Ch1.T1"/>) in order to determine local and
diurnal trends in PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> and to determine the extent to
which remotely sensed measurements of atmospheric particulates are able to
capture trends in PM concentrations that are observed at the ground in
densely populated urban areas. When seasonal characteristics are described,
southern hemisphere summer is defined as December–February (DJF), fall is
March–May (MAM), winter is June–August (JJA), and spring is
September–November (SON).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><caption><p>Map depicting satellite study grids, with a summary of area and point sources.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f01.png"/>

      </fig>

<sec id="Ch1.S2.SS1">
  <title>Remotely sensed aerosol data</title>
      <p>Remotely sensed aerosol data from Moderate Resolution Imaging
Spectroradiometer (MODIS) Version 5.1 <xref ref-type="bibr" rid="bib1.bibx50" id="paren.15"/>, Multi-angle Imaging
Spectroradiometer (MISR) Version 31 <xref ref-type="bibr" rid="bib1.bibx15 bib1.bibx14" id="paren.16"/>, and
Total Ozone Mapping Spectrometer (TOMS) Version 8 <xref ref-type="bibr" rid="bib1.bibx25" id="paren.17"/> were
obtained from NASA's Giovanni Data and Information Services Center
(<uri>http://disc.sci.gsfc.nasa.gov/giovanni</uri>). Data from MODIS included
1 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> gridded cloud fraction, aerosol optical depth (AOD
or <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">τ</mml:mi></mml:math></inline-formula>) at 550 nm from both MODIS Aqua and Terra platforms (AOD<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>550</mml:mn></mml:msub></mml:math></inline-formula>),
and Ångström Exponent (<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>) with MODIS Aqua representing
spectral dependence of AOD between <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>=</mml:mo></mml:mrow></mml:math></inline-formula> 550 and 865 nm and MODIS Terra
between <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>=</mml:mo></mml:mrow></mml:math></inline-formula> 470 and 660 nm. MODIS data were available between
1 March 2000 and 31 December 2009 (Terra) and 4 July 2002 and 31 December 2009
(Aqua). We utilized daily 1 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> gridded Deep Blue AOD
(550 nm) from MODIS <xref ref-type="bibr" rid="bib1.bibx28" id="paren.18"/>, which is based on a retrieval algorithm
capable of distinguishing particles over bright land surfaces and returning
AODs within 20–30 % of ground-based sun photometers <xref ref-type="bibr" rid="bib1.bibx29" id="paren.19"/>. AOD at
555 nm (AOD<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>555</mml:mn></mml:msub></mml:math></inline-formula>) and resolution of 0.5 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.5<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> were
obtained from MISR for the period 25 February 2000 to 31 December 2009. Ultraviolet
Aerosol Index at 1 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1.25<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> was obtained from TOMS for the
period 24 February 2000 to 14 December 2005, utilizing a minimum UVAI threshold of 0.5
to account for retrieval uncertainties. For all remotely sensed data, a
filter was applied to use only data corresponding to cloud fraction <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="italic">&lt;</mml:mi><mml:mn> 70</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="italic">%</mml:mi></mml:mrow></mml:math></inline-formula>.</p>
</sec>
<sec id="Ch1.S2.SS2">
  <title>Goddard Ozone Chemistry Aerosol Radiation and Transport (GOCART) model</title>
      <p>Data from the Goddard Ozone Chemistry Aerosol Radiation and Transport model
<xref ref-type="bibr" rid="bib1.bibx10" id="paren.20"><named-content content-type="pre">GOCART;</named-content></xref> were used to determine modeled contribution to
total AOD<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>550</mml:mn></mml:msub></mml:math></inline-formula> by individual aerosol components: black carbon, organic
carbon, dust, sulfate, and sea salt. Resolution was 2 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 2.5<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> and data were obtained from NASA's Giovanni Data and
Information Services Center for the period between 24 February 2000 and
31 December 2007.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><caption><p>Ground-based air quality monitoring sites in the Gauteng area.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="5">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:colspec colnum="5" colname="col5" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Site</oasis:entry>  
         <oasis:entry colname="col2">Network</oasis:entry>  
         <oasis:entry colname="col3">Type</oasis:entry>  
         <oasis:entry colname="col4">Data</oasis:entry>  
         <oasis:entry colname="col5">Date Range</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">Alexandra</oasis:entry>  
         <oasis:entry colname="col2">Johannesburg</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 Jan 2004 to 31 Oct 2010</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Jabavu (Soweto)</oasis:entry>  
         <oasis:entry colname="col2">Johannesburg</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">14 Jul 2004 to 20 May 2011</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Orange Farm</oasis:entry>  
         <oasis:entry colname="col2">Johannesburg</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">17 May 2004 to 1 Jun 2011</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Delta Park</oasis:entry>  
         <oasis:entry colname="col2">Johannesburg</oasis:entry>  
         <oasis:entry colname="col3">Urban/Suburban Residential</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">31 Jul 2004 to 9 Dec 2010</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Newtown</oasis:entry>  
         <oasis:entry colname="col2">Johannesburg</oasis:entry>  
         <oasis:entry colname="col3">Urban/Suburban Residential</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">31 Jul 2004 to 1 Jun 2011</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Buccleuch</oasis:entry>  
         <oasis:entry colname="col2">Johannesburg</oasis:entry>  
         <oasis:entry colname="col3">Traffic</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula>, PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">31 Jul 2004 to 1 Jun 2011</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Bodibeng</oasis:entry>  
         <oasis:entry colname="col2">Tshwane</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 May 2012 to 28 Feb 2014</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Olivienhoutbosch</oasis:entry>  
         <oasis:entry colname="col2">Tshwane</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 May 2012 to 31 Dec 2013</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Pretoria (PTA) West</oasis:entry>  
         <oasis:entry colname="col2">Tshwane</oasis:entry>  
         <oasis:entry colname="col3">Industrial</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">25 Jun 2012 to 5 Oct 2014</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Rosslyn</oasis:entry>  
         <oasis:entry colname="col2">Tshwane</oasis:entry>  
         <oasis:entry colname="col3">Industrial</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">20 Jun 2012 to 6 Mar 2014</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Ekandustria</oasis:entry>  
         <oasis:entry colname="col2">Tshwane</oasis:entry>  
         <oasis:entry colname="col3">Industrial</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 Sep 2012 to 21 Feb 2014</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Booysens</oasis:entry>  
         <oasis:entry colname="col2">Tshwane</oasis:entry>  
         <oasis:entry colname="col3">Urban/Suburban Residential</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 May 2012 to 28 Feb 2014</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Etwatwa</oasis:entry>  
         <oasis:entry colname="col2">Ekurhuleni</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 Jan 2011 to 30 Sep 2012</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Tembisa</oasis:entry>  
         <oasis:entry colname="col2">Ekurhuleni</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 Jul 2011 to 30 Sep 2011</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Diepkloof</oasis:entry>  
         <oasis:entry colname="col2">VTAPA</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula>, PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 Feb 2007 to 31 Dec 2012</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Sebokeng</oasis:entry>  
         <oasis:entry colname="col2">VTAPA</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula>, PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 Feb 2007 to 31 Dec 2012</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Sharpeville</oasis:entry>  
         <oasis:entry colname="col2">VTAPA</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula>, PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 Mar 2007 to 31 Dec 2012</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Zamdela</oasis:entry>  
         <oasis:entry colname="col2">VTAPA</oasis:entry>  
         <oasis:entry colname="col3">Township/Domestic Burning</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula>, PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 Mar 2007 to 31 Dec 2012</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Three Rivers</oasis:entry>  
         <oasis:entry colname="col2">VTAPA</oasis:entry>  
         <oasis:entry colname="col3">Industrial</oasis:entry>  
         <oasis:entry colname="col4">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula>, PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col5">1 Feb 2007 to 31 Dec 2012</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

</sec>
<sec id="Ch1.S2.SS3">
  <title>Satellite fire data</title>
      <p>Data from the MODIS Fire Information for Resource Management System (FIRMS;
<uri>https://earthdata.nasa.gov/data/near-real-time-data/firms/active-fire-data#tab-content-6</uri>)
provided a climatology of burn frequency and intensity over southern Africa
(0 to 35<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and 5 to 55<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) between 1 January 2000 and
31 December 2009. FIRMS data are available for each MODIS overpass and lists the
location of identified fires along with fire characteristics which includes
fire radiative power (FRP), which captures the intensity of burning within
each fire pixel. To capture the frequency and geographical range of burning
together with intensity, we report time average FRP integrated at a
resolution of 0.5 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.5<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>.</p>
</sec>
<sec id="Ch1.S2.SS4">
  <title>Air-mass back-trajectory data</title>
      <p>NOAA's Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT)
model <xref ref-type="bibr" rid="bib1.bibx16" id="paren.21"/> was run using NCAR/NCEP reanalysis data with the
isentropic vertical velocity method in order to determine air-mass origin for
the Gauteng satellite grid box. Trajectories were obtained from 1 January 2000
through 31 December 2009 ending at the center of the box (26<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S,
28<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) at 500 m above the surface. Seasonal trajectory frequency
maps were constructed for fall (March–May), winter (June–August), spring (September–November),
and summer (December–February) in order to illustrate the most frequent source areas
for air arriving in the Gauteng region and aid in interpreting combined
satellite and ground results for the region.</p>
</sec>
<sec id="Ch1.S2.SS5">
  <title>Ground data</title>
      <p>Hourly ground-based air quality data were obtained from four different
networks reporting to the South African Air Quality Information System
(SAAQIS), all located within the Gauteng satellite grid box. Table <xref ref-type="table" rid="Ch1.T1"/> categorizes individual ground monitoring sites
according to both the monitoring network and site type to which they belong,
and gives date ranges and data available. Site classifications were made on
the basis of site descriptions on the SAAQIS website (available at
<uri>http://www.saaqis.org.za/NAAQM.aspx</uri>), site visits, and personal
correspondence with the NGO NOVA Institute, which works extensively in
townships and informal settlements. Data were used as per approval from each
monitoring network, and were subject to data quality controls. Negative
values were discarded, as well as “repeat” values with the same value given
for many hours at a time. Where &gt; 30 % of data points were missing over a
given time-averaging period, data were discarded.</p>
      <p>Ground-based aerosol optical depth and Ångström Exponent are
available from multiple Gauteng-area sites in the Aerosol Robotic Network
(AERONET). A comparison of ground-based and remotely sensed column aerosol
parameters is beyond the scope of this work, but will be presented in a
separate publication.</p>
</sec>
<sec id="Ch1.S2.SS6">
  <title>Meteorology Data</title>
      <p>Hourly ground-based meteorology observations were obtained through the South
African Weather Service (SAWS) for five sites corresponding to each of the
five major metropolitan study areas considered in the study. Data include
pressure, precipitation, temperature, relative humidity, wind direction, and
wind speed from Cape Town (33.98<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S, 18.60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E; 1 April 2001
through 31 December 2009), Bloemfontein (29.12<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S, 26.19<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E;
25 December 2000 through 31 December 2009), Johannesburg (26.15<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S,
28.00<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E; 25 December 2000 through 31 December 2009), Ermelo (26.50<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S, 29.98<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E; 25 December 2000 through 31 December 2009) and Durban
(29.97<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S, 30.95<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E; 25 December 2000 through 31 December 2009).</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <title>Results and discussion</title>
<sec id="Ch1.S3.SS1">
  <title>Study areas: land use and emissions</title>
      <p>Locations and sizes of study areas are displayed in
Fig. <xref ref-type="fig" rid="Ch1.F1"/>. Zoom-in outsets show land use percentage and major
emissions sources for each region. In every region there are significant area
sources corresponding to biomass burning (veld fires that occur in early to
mid-winter) and informal settlements (primarily domestic burning throughout
the winter). Mine tailings and waste dumps from gold mining are prevalent in
Gauteng, with emissions dependent on wind speed. Petroleum refineries are
major point sources in Gauteng, HVAPA and Durban, with some presence in Cape
Town. Coal-fired power plants are prevalent through Gauteng and HVAPA, and
are collocated with open mining along coal deposits in the region. Overall,
Gauteng and HVAPA have by far the highest density of anthropogenic emissions
from all sources, including significant on-road emissions.</p>
</sec>
<sec id="Ch1.S3.SS2">
  <title>Satellite and model results</title>
      <p>A number of satellite and model products are available through NASA's
Giovanni Data and Information Services Center
(<uri>http://disc.sci.gsfc.nasa.gov/giovanni</uri>). We focus here on products
related to atmospheric particulates, presenting decadal averages (1 January
2000 to 31 December 2009 or some multi-year subset, depending on data
availability) of Aerosol Optical Depth (AOD or <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">τ</mml:mi></mml:math></inline-formula>), Ångström
Exponent (<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>), Ultraviolet Aerosol Index (UVAI), and chemical component
contributions to AOD from The Goddard Chemistry Aerosol Radiation and
Transport (GOCART) model. Each of these parameters describes a unique aspect
of the aerosol column, and results will be presented as follows: (i) a brief
description of the parameter, (ii) general regional and seasonal trends, and
(iii) discussion of those trends, incorporating other data platforms to
support conclusions where appropriate. Main conclusions are synthesized in
Sect. <xref ref-type="sec" rid="Ch1.S4"/>, and satellite data are summarized in
Table <xref ref-type="table" rid="Ch1.T2"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><caption><p>AOD averages for each region for the period 1 January 2000 to 31 December 2009. Error bars represent one standard deviation in the mean.</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f02.pdf"/>

        </fig>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T2" specific-use="star"><caption><p>Seasonal averages of satellite data from the MODIS-Aqua, MODIS-Terra, and MISR platforms for each region and as a South Africa average, for the period 1 January 2000 to 31 December 2009.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="7">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:colspec colnum="5" colname="col5" align="left"/>
     <oasis:colspec colnum="6" colname="col6" align="left"/>
     <oasis:colspec colnum="7" colname="col7" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Parameter</oasis:entry>  
         <oasis:entry colname="col2">Region</oasis:entry>  
         <oasis:entry colname="col3">Platform</oasis:entry>  
         <oasis:entry colname="col4">Summer</oasis:entry>  
         <oasis:entry colname="col5">Fall</oasis:entry>  
         <oasis:entry colname="col6">Winter</oasis:entry>  
         <oasis:entry colname="col7">Spring</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">AOD</oasis:entry>  
         <oasis:entry colname="col2">CPT</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">0.07 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01</oasis:entry>  
         <oasis:entry colname="col5">0.06 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col6">0.05 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01</oasis:entry>  
         <oasis:entry colname="col7">0.19 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">0.08 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col5">0.06 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col6">0.06 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01</oasis:entry>  
         <oasis:entry colname="col7">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">MISR</oasis:entry>  
         <oasis:entry colname="col4">0.11 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col5">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.18</oasis:entry>  
         <oasis:entry colname="col6">0.10 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.14 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08</oasis:entry>  
         <oasis:entry colname="col5">0.08 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.10</oasis:entry>  
         <oasis:entry colname="col6">0.07 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col7">0.15 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">Bloemfontein</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">0.10 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col5">0.08 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col6">0.10 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col7">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col5">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col6">0.10 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">MISR</oasis:entry>  
         <oasis:entry colname="col4">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col5">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col6">0.08 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col7">0.16 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">0.11 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col5">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col6">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.14 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">Johannesburg/PTA</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col5">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col6">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col7">0.17 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.06</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">0.15  <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col5">0.14 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col6">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.17 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">MISR</oasis:entry>  
         <oasis:entry colname="col4">0.18 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>  
         <oasis:entry colname="col5">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col6">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col7">0.21 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">0.15 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col5">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col6">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col7">0.18 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">HVAPA</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">0.15 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col5">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col6">0.11 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.19 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.06</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">0.08 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col5">0.08 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col6">0.10 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col7">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">MISR</oasis:entry>  
         <oasis:entry colname="col4">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col5">0.08 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col6">0.08 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.14 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col5">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col6">0.10 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.15 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">Durban</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col5">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col6">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.14 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col5">0.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02</oasis:entry>  
         <oasis:entry colname="col6">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.15 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">MISR</oasis:entry>  
         <oasis:entry colname="col4">0.18 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09</oasis:entry>  
         <oasis:entry colname="col5">0.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>  
         <oasis:entry colname="col6">0.18 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>  
         <oasis:entry colname="col7">0.24 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.06</oasis:entry>  
         <oasis:entry colname="col5">0.11 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col6">0.15 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.04</oasis:entry>  
         <oasis:entry colname="col7">0.18 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">South Africa</oasis:entry>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">0.12 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>  
         <oasis:entry colname="col5">0.10 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>  
         <oasis:entry colname="col6">0.11 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03</oasis:entry>  
         <oasis:entry colname="col7">0.16 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"><inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2">CPT</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">1.19 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09</oasis:entry>  
         <oasis:entry colname="col5">1.26 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11</oasis:entry>  
         <oasis:entry colname="col6">1.21 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.12</oasis:entry>  
         <oasis:entry colname="col7">1.39 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.10</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">1.25 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.12</oasis:entry>  
         <oasis:entry colname="col5">1.39 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.14</oasis:entry>  
         <oasis:entry colname="col6">1.40 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col7">0.97 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">1.22 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.10</oasis:entry>  
         <oasis:entry colname="col5">1.33 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.12</oasis:entry>  
         <oasis:entry colname="col6">1.31 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col7">1.18 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">Bloemfontein</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">1.18 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.32</oasis:entry>  
         <oasis:entry colname="col5">0.90 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.20</oasis:entry>  
         <oasis:entry colname="col6">0.67 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.06</oasis:entry>  
         <oasis:entry colname="col7">0.92 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.22</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">0.99 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.34</oasis:entry>  
         <oasis:entry colname="col5">0.82 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.19</oasis:entry>  
         <oasis:entry colname="col6">0.70 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11</oasis:entry>  
         <oasis:entry colname="col7">0.92 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.30</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">1.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.33</oasis:entry>  
         <oasis:entry colname="col5">0.86 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.19</oasis:entry>  
         <oasis:entry colname="col6">0.69 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09</oasis:entry>  
         <oasis:entry colname="col7">0.92 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.26</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">Johannesburg/PTA</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">1.26 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.28</oasis:entry>  
         <oasis:entry colname="col5">0.86 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.12</oasis:entry>  
         <oasis:entry colname="col6">0.69 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08</oasis:entry>  
         <oasis:entry colname="col7">0.95 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.29</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">1.20 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.22</oasis:entry>  
         <oasis:entry colname="col5">0.88 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.15</oasis:entry>  
         <oasis:entry colname="col6">0.80 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.19</oasis:entry>  
         <oasis:entry colname="col7">1.16 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.34</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">1.23 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.25</oasis:entry>  
         <oasis:entry colname="col5">0.87 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col6">0.75 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.15</oasis:entry>  
         <oasis:entry colname="col7">1.06 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.31</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">HVAPA</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">1.13 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.35</oasis:entry>  
         <oasis:entry colname="col5">0.95 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.25</oasis:entry>  
         <oasis:entry colname="col6">0.69 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.07</oasis:entry>  
         <oasis:entry colname="col7">0.97 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.27</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">1.22 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.23</oasis:entry>  
         <oasis:entry colname="col5">0.79 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.19</oasis:entry>  
         <oasis:entry colname="col6">0.71 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08</oasis:entry>  
         <oasis:entry colname="col7">1.39 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.24</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">1.18 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.30</oasis:entry>  
         <oasis:entry colname="col5">0.87 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.22</oasis:entry>  
         <oasis:entry colname="col6">0.70 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.08</oasis:entry>  
         <oasis:entry colname="col7">1.18 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.25</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">Durban</oasis:entry>  
         <oasis:entry colname="col3">Aqua</oasis:entry>  
         <oasis:entry colname="col4">1.50 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col5">1.33 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.10</oasis:entry>  
         <oasis:entry colname="col6">1.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11</oasis:entry>  
         <oasis:entry colname="col7">1.68 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Terra</oasis:entry>  
         <oasis:entry colname="col4">1.40 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.12</oasis:entry>  
         <oasis:entry colname="col5">1.29 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11</oasis:entry>  
         <oasis:entry colname="col6">1.08 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.15</oasis:entry>  
         <oasis:entry colname="col7">1.61 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.10</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">1.45 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col5">1.31 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11</oasis:entry>  
         <oasis:entry colname="col6">1.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col7">1.65 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">South Africa</oasis:entry>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">1.23 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.24</oasis:entry>  
         <oasis:entry colname="col5">1.05 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.16</oasis:entry>  
         <oasis:entry colname="col6">0.90 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.12</oasis:entry>  
         <oasis:entry colname="col7">1.20 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.23</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">UVAI</oasis:entry>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">CPT</oasis:entry>  
         <oasis:entry colname="col4">1.09 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.28</oasis:entry>  
         <oasis:entry colname="col5">0.73 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.10</oasis:entry>  
         <oasis:entry colname="col6">0.74 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09</oasis:entry>  
         <oasis:entry colname="col7">0.95 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.21</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Bloemfontein</oasis:entry>  
         <oasis:entry colname="col4">0.96 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.30</oasis:entry>  
         <oasis:entry colname="col5">0.74 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col6">0.75 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.17</oasis:entry>  
         <oasis:entry colname="col7">0.95 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.23</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Johannesburg/PTA</oasis:entry>  
         <oasis:entry colname="col4">0.94 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.29</oasis:entry>  
         <oasis:entry colname="col5">0.76 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col6">0.75 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.15</oasis:entry>  
         <oasis:entry colname="col7">0.97 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.24</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">HVAPA</oasis:entry>  
         <oasis:entry colname="col4">0.98 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.29</oasis:entry>  
         <oasis:entry colname="col5">0.73 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.13</oasis:entry>  
         <oasis:entry colname="col6">0.75 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.18</oasis:entry>  
         <oasis:entry colname="col7">0.95 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.22</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Durban</oasis:entry>  
         <oasis:entry colname="col4">1.01 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.27</oasis:entry>  
         <oasis:entry colname="col5">0.72 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11</oasis:entry>  
         <oasis:entry colname="col6">0.80 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.20</oasis:entry>  
         <oasis:entry colname="col7">0.95 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.24</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">South Africa</oasis:entry>  
         <oasis:entry colname="col3">Average</oasis:entry>  
         <oasis:entry colname="col4">1.00 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.29</oasis:entry>  
         <oasis:entry colname="col5">0.74 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.12</oasis:entry>  
         <oasis:entry colname="col6">0.76 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.17</oasis:entry>  
         <oasis:entry colname="col7">0.95 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.22</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

<sec id="Ch1.S3.SS2.SSS1">
  <title>Aerosol Optical Depth (AOD)</title>
      <p>AOD<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>550</mml:mn></mml:msub></mml:math></inline-formula> from the MODIS (Aqua and Terra) and AOD<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>555</mml:mn></mml:msub></mml:math></inline-formula> MISR satellite
platforms, and total AOD predicted by GOCART are presented in
Fig. <xref ref-type="fig" rid="Ch1.F2"/>. AOD is a measure of the reduction of intensity of light
due to scattering and absorption of particles along path length, and is
defined for a specific height (<inline-formula><mml:math display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula>) and wavelength (<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">λ</mml:mi></mml:math></inline-formula>) according to
the Beer–Lambert law:
              <disp-formula id="Ch1.E1" content-type="numbered"><mml:math display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi>F</mml:mi><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>,</mml:mo><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>)</mml:mo></mml:mrow><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">TOA</mml:mi></mml:msub><mml:mo>(</mml:mo><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mi>exp⁡</mml:mi><mml:mo>(</mml:mo><mml:mo>-</mml:mo><mml:mi mathvariant="italic">τ</mml:mi><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>,</mml:mo><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>)</mml:mo><mml:mo>)</mml:mo><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
            where transmittance, or <inline-formula><mml:math display="inline"><mml:mfrac><mml:mrow><mml:mi>F</mml:mi><mml:mo>(</mml:mo><mml:mi>z</mml:mi><mml:mo>,</mml:mo><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>)</mml:mo></mml:mrow><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">TOA</mml:mi></mml:msub><mml:mo>(</mml:mo><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:mfrac></mml:math></inline-formula>, is the
ratio of radiation intensity at height <inline-formula><mml:math display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula> to intensity at the top of
atmosphere (TOA), for a given wavelength <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">λ</mml:mi></mml:math></inline-formula>. Here, <inline-formula><mml:math display="inline"><mml:mi>z</mml:mi></mml:math></inline-formula> is the entire
atmosphere path length between the ground and TOA, and <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">λ</mml:mi></mml:math></inline-formula> is 550 nm
for both MODIS platforms (Aqua and Terra) and 555 nm for MISR. For
simplicity, MISR AOD (555 nm) has been converted to equivalent AOD<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>550</mml:mn></mml:msub></mml:math></inline-formula>
<xref ref-type="bibr" rid="bib1.bibx54" id="paren.22"><named-content content-type="pre">e.g.,</named-content></xref> and simply referred to as AOD. AOD is a function
of particle extinction efficiency (<inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>Q</mml:mi><mml:mtext>ext</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>), which depends on both
particle size and absorption efficiency, and particle number concentration.
Low values of AOD (<inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="italic">&lt;</mml:mi><mml:mn> 0.1</mml:mn></mml:mrow></mml:math></inline-formula>) correspond to little light attenuation through
the atmosphere – meaning relatively clean conditions with low particle
concentrations, few large particles, and aerosol number distributions
comprised primarily of small, non-absorbing particles. High values of AOD
(&gt; 0.3) correspond to significant light attenuation in the atmosphere
– meaning high concentrations of large particles such as dust, high
concentrations of absorbing aerosol such as black carbon at any size, or some
combination of the two. Typical values of AOD range from 0.05 in remote,
clean environments to 1.0 in areas of extreme particle concentrations
<xref ref-type="bibr" rid="bib1.bibx55" id="paren.23"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><caption><p>Monthly averaged FRP integrated over 0.5 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.5<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>
boxes in the Southern Africa Domain over the period 1 January 2000 to 31 December 2009 from MODIS thermal anomaly retrieval.</p></caption>
            <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f03.pdf"/>

          </fig>

      <p>Discrepancies in AOD between satellite platforms are generally within
uncertainty, and arise due to differences in factors such as processing
methods <xref ref-type="bibr" rid="bib1.bibx1" id="paren.24"/>, calibration and retrieval algorithms
<xref ref-type="bibr" rid="bib1.bibx30" id="paren.25"/>, and even measurement time (MODIS-Terra and MISR pass over
South Africa between 09:00 and 11:00 LT, while MODIS-Aqua passes over between
13:00 and 15:00 LT). In this study, AOD from MODIS Aqua and Terra are
well-correlated with AOD from MISR, with Pearson's <inline-formula><mml:math display="inline"><mml:mi>R</mml:mi></mml:math></inline-formula> correlation coefficients
<inline-formula><mml:math display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mi>r</mml:mi><mml:mo>)</mml:mo><mml:mi mathvariant="italic">&gt;</mml:mi><mml:mn>0.7</mml:mn></mml:mrow></mml:math></inline-formula> (not shown), except in Cape Town and Bloemfontein (<inline-formula><mml:math display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>=</mml:mo><mml:mn>0.36</mml:mn></mml:mrow></mml:math></inline-formula> and
0.59, respectively). Total AOD modeled by GOCART correlates well with all
satellite platforms in all sites (<inline-formula><mml:math display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mi mathvariant="italic">&gt;</mml:mi><mml:mn>0.7</mml:mn></mml:mrow></mml:math></inline-formula>). In Cape Town and Durban, MISR
AOD appears significantly higher than either MODIS platform or GOCART. The
surface at both of these sites displays a great deal of heterogeneity, with
satellite grid boxes extending over both bright land and dark ocean surfaces.
While estimated biases between MISR and MODIS are expected to be low over
uniformly dark surfaces <xref ref-type="bibr" rid="bib1.bibx30" id="paren.26"/>, assumptions about surface
reflectivity tend to introduce significant discrepancies with increased
surface heterogeneity <xref ref-type="bibr" rid="bib1.bibx11" id="paren.27"/>. MISR is less sensitive to surface
characteristics, and so in regions with significant heterogeneity such as
Cape Town or Durban, one may expect AOD from MISR to be more accurate.</p>
      <p>Considering Fig. <xref ref-type="fig" rid="Ch1.F2"/>, AOD is consistently lower in Cape Town than
other major metropolitan areas of South Africa, owing to frequent air-mass
origin over clean marine areas and minor influence by large or absorbing
aerosols. At continentally influenced sites (Bloemfontein, Gauteng, HVAPA,
and Durban), there is a maximum in AOD between 0.12 and 0.20 from late winter
to early spring. AOD is moderate through summer, averaging 0.08–0.17, and
reaches a minimum during late fall and early winter (MJJ), with AOD ranging
from 0.05–0.10. AOD is particularly high in magnitude and variability in
Durban between August and October, with MISR AOD showing monthly averages
approaching 0.3. The seasonal trends evident in Fig. <xref ref-type="fig" rid="Ch1.F2"/> can be
explained by considering annual variability in (1) biomass burning and (2)
dust generation. The impact of these parameters on AOD is explored below.</p>
      <p>The first and most distinct annual feature across South African metropolitan
areas is the cycle in AOD, from minima during late spring and early winter
(May–July) to maxima from August to October. This maximum coincides with the
burning season in Southern Africa, which has been identified as major
regional source of transported aerosol in South Africa <xref ref-type="bibr" rid="bib1.bibx45 bib1.bibx46 bib1.bibx21 bib1.bibx22 bib1.bibx17 bib1.bibx53 bib1.bibx6 bib1.bibx57 bib1.bibx43 bib1.bibx66 bib1.bibx39 bib1.bibx48" id="paren.28"/>. Figure <xref ref-type="fig" rid="Ch1.F3"/> presents average monthly integrated
fire radiative power (FRP) per km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> from 2000–2010 in Sub-Saharan
Africa, and indicates that the most significant burning in Southern Africa
occurs between May and September and is located in the tropics (between 0 and
20<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S). These fires are massive sources of biomass burning emissions
that are often transported in stratified layers aloft <xref ref-type="bibr" rid="bib1.bibx6" id="paren.29"/>,
and this transport significantly impacts aerosol optical properties in South
Africa <xref ref-type="bibr" rid="bib1.bibx21 bib1.bibx57 bib1.bibx43 bib1.bibx39" id="paren.30"/>.</p>
      <p>Winkler et al. (<xref ref-type="bibr" rid="bib1.bibx66" id="year.31"/>) demonstrated that transported
biomass burning emissions represent the dominant source of irradiation losses
during late winter and early spring in South Africa, with the majority of
scattering attributable to carbonaceous aerosols <xref ref-type="bibr" rid="bib1.bibx40" id="paren.32"/>. Queface
et al. (<xref ref-type="bibr" rid="bib1.bibx48" id="year.33"/>) indicated that transported fire emissions
represent the bulk of column aerosol loading between August and October.
Strong north-to-south gradients in AOD are observed during the burning
season, with significantly higher AOD near sources, where aerosols are small,
but highly absorbing and concentrated <xref ref-type="bibr" rid="bib1.bibx17 bib1.bibx6 bib1.bibx38 bib1.bibx49 bib1.bibx39" id="paren.34"/>. Lower AOD is typically observed at downwind
receptor sites after plumes have evolved to comprise less absorbing and
predominantly Aitken and accumulation mode particles with sufficient
condensed water-soluble secondary aerosol species for the particles to serve
as cloud condensation nuclei (CCN) <xref ref-type="bibr" rid="bib1.bibx53 bib1.bibx17 bib1.bibx57 bib1.bibx49 bib1.bibx8 bib1.bibx39" id="paren.35"/>.</p>
      <p>On the basis of strong N–S gradients in biomass-burning-related AOD, and the
finding that AOD is highest nearest sources (above), it follows that AOD in
South Africa is enhanced most significantly by close-proximity fires within
South African borders and in neighboring Mozambique and Zimbabwe. These
close-proximity fires reach their peak frequency in August, September, and
October and coincide with the maxima in AOD observed across all
continentally influenced sites in this study. Because AOD is highest in
closest proximity to fires, the influence of biomass burning on AOD is
expected to be strongest nearer sources in eastern South Africa. Proximity
explains the high magnitude and variability of AOD in Durban between August
and October, where very close proximity sugar cane field burning typically
occurs, releasing high and variable concentrations of absorbing biomass
burning particles <xref ref-type="bibr" rid="bib1.bibx33" id="paren.36"/>. Periodically compounding the impact
of proximity in eastern South Africa is the so-called “river of smoke”
phenomenon <xref ref-type="bibr" rid="bib1.bibx3" id="paren.37"/>, whereby synoptic air flows are occasionally
favorable for the transport of subtropical biomass burning into a narrow
latitudinal region over the northeastern part of the country – the area that
is also closest to high frequency and intensity of seasonal fires.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><caption><p>Monthly averaged values of RH, accumulated rainfall, wind speed, and
temperature for sites in each satellite study area for the period 1 January 2000
to 31 December 2009. Note different <inline-formula><mml:math display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> scales for each site.</p></caption>
            <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f04.pdf"/>

          </fig>

      <p>In addition to coinciding with biomass burning, elevated AOD in August and
September is correlated with enhanced generation of windblown dust across
South Africa. Ground-based meteorology data from South African Weather
Service (SAWS) monitoring sites in each region are presented in
Fig. <xref ref-type="fig" rid="Ch1.F4"/>, and indicate that in all regions but Cape Town,
wind speeds increase in July and August before an enhancement in
precipitation in September and October. High winds combined with dry
conditions result in generation of wind-blown dust particles, which are both
large and strongly absorbing and thereby have strong bearing on AOD. Enhanced
AOD coincides with dust generation during August and September, and we
therefore suggest that dust may be an additional, previously underestimated
factor influencing AOD across South Africa.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><caption><p>Average monthly column water vapor (CWV, black line) for the period
1 January 2000 to 31 December 2009, with gray shading representing minimum and
maximum monthly CWV during that period.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f05.pdf"/>

          </fig>

      <p>Column water vapor (CWV; Fig. <xref ref-type="fig" rid="Ch1.F5"/>) derived from the Modern
Era-Retrospective Analysis for Research and Applications
<xref ref-type="bibr" rid="bib1.bibx51" id="paren.38"><named-content content-type="pre">MERRA;</named-content></xref> was analyzed for each site in order to
determine whether enhanced water vapor might be a factor contributing to
elevated AOD through a mechanism of hygroscopic growth of particles. No significant correlation was found between AOD and CWV at any site,
supporting findings in Kumar et al. (<xref ref-type="bibr" rid="bib1.bibx32" id="year.39"/>), which found no
relationship between AOD and CWV at a site in rural, northeastern South
Africa.</p>
      <p>Overall, AOD values reported here are consistent with those reported by
Tesfaye et al. (<xref ref-type="bibr" rid="bib1.bibx60" id="year.40"/>) based on broad, regionally averaged
10-year MISR AOD trends for northern, central, and southern regions of South
Africa. The observation of enhanced AOD associated with transported biomass
burning aerosol also agrees with similar trends for central and northern
South Africa in that work. But overall, AOD is lower than many
previously published values over Southern Africa. Queface et al. (<xref ref-type="bibr" rid="bib1.bibx48" id="year.41"/>) reported long-term, monthly averaged AOD ranging
from 0.10 to over 0.60 at a site near dense biomass burning sources in Zambia,
and monthly averages between 0.17 and 0.30 at a site in northeastern South
Africa near the Mozambique border. A strong N–S gradient in AOD is typically
observed during biomass burning season in Southern Africa <xref ref-type="bibr" rid="bib1.bibx17" id="paren.42"/>,
with sites to the north experiencing significantly higher AOD than sites in
the south due to closer proximity to sources. This suggests that while
transported biomass burning aerosol has a clear impact on AOD across the
major metropolitan areas of South Africa (except Cape Town), this impact is
nonetheless much less pronounced than for sites farther to the north and
closer to denser burning sources.</p>
      <p>As AOD is frequently used as a proxy for megacity anthropogenic particulate
pollution, it is important to view results from South Africa within the
context of worldwide megacities. Considering the major metropolitan and
industrial areas of Gauteng and HVAPA, seasonally averaged AOD ranged from a
minimum of 0.12 in winter to a maximum of 0.17 in spring – values that are a
factor of 3–6 lower than those typical of megacities and major industrial
areas worldwide. Annual averages of AOD in industrialized and urban areas of
Hong Kong and China such as Nanjing, the North China Plain, and Yangtze
River are on the order of 0.6–0.8 <xref ref-type="bibr" rid="bib1.bibx69 bib1.bibx36 bib1.bibx68" id="paren.43"/>. AOD in Mexico City ranges from a seasonally averaged minimum of
0.2 to a maximum of 0.6 <xref ref-type="bibr" rid="bib1.bibx42" id="paren.44"/>, and in the Dheli region of India
AOD ranges from a seasonal minimum of 0.4 to a maximum during monsoon season
of 1.4. So while the Gauteng area and HVAPA areas are characterized as
a megacity on the basis of remotely sensed column NO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula>
<xref ref-type="bibr" rid="bib1.bibx4 bib1.bibx35" id="paren.45"/>, AOD is significantly lower than typical
megacity areas.</p>
</sec>
<sec id="Ch1.S3.SS2.SSS2">
  <?xmltex \opttitle{{\AA}ngstr{\"{o}}m exponent ($\alpha$)}?><title>Ångström exponent (<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>)</title>
      <p>Monthly averaged Ångström exponent (<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>) from the MODIS Aqua and
Terra platforms is presented in Fig. <xref ref-type="fig" rid="Ch1.F6"/>. <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> captures
the spectral dependence of aerosol extinction based on measurements of AOD at
two different wavelengths:
              <disp-formula id="Ch1.E2" content-type="numbered"><mml:math display="block"><mml:mrow><mml:mi mathvariant="italic">α</mml:mi><mml:mo>=</mml:mo><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>log⁡</mml:mi><mml:mi mathvariant="italic">τ</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>log⁡</mml:mi><mml:mi mathvariant="italic">λ</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi>log⁡</mml:mi><mml:mo>(</mml:mo><mml:mfrac><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:mfrac><mml:mo>)</mml:mo></mml:mrow><mml:mrow><mml:mi>log⁡</mml:mi><mml:mo>(</mml:mo><mml:mfrac><mml:mrow><mml:msub><mml:mi mathvariant="italic">λ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mi mathvariant="italic">λ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:mfrac><mml:mo>)</mml:mo></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
            where <inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> are AODs at wavelengths <inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">λ</mml:mi><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula>. For
small particles in the Rayleigh scattering regime (<inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi>p</mml:mi></mml:msub><mml:mi mathvariant="italic">&lt;</mml:mi><mml:mn>0.1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m), AOD
scales with wavelength as (<inline-formula><mml:math display="inline"><mml:mfrac><mml:mn mathvariant="normal">1</mml:mn><mml:mrow><mml:msup><mml:mi mathvariant="italic">λ</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:mrow></mml:mfrac></mml:math></inline-formula> to <inline-formula><mml:math display="inline"><mml:mfrac><mml:mn mathvariant="normal">1</mml:mn><mml:mrow><mml:msup><mml:mi mathvariant="italic">λ</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msup></mml:mrow></mml:mfrac></mml:math></inline-formula>), and <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="italic">α</mml:mi><mml:mi mathvariant="italic">&gt;</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>
where fine particles dominate. Large particles, on the other hand, are more
spectrally neutral and the lack of wavelength dependence of scattering and
absorption results in <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mi mathvariant="italic">&lt;</mml:mi><mml:mi mathvariant="italic">α</mml:mi><mml:mi mathvariant="italic">&lt;</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> where coarse particles dominate.
<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> is reported for both MODIS platforms, with Aqua representing
spectral dependence of AOD between <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>=</mml:mo><mml:mn>550</mml:mn></mml:mrow></mml:math></inline-formula> and 865 nm and Terra
between <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="italic">λ</mml:mi><mml:mo>=</mml:mo><mml:mn>470</mml:mn></mml:mrow></mml:math></inline-formula> and 660 nm.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6"><caption><p>Monthly averaged values of Ångström Exponent (<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>) for each region for the period 1 January 2000 to 31 December 2009.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f06.pdf"/>

          </fig>

      <p><inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> is quantized in such a way that it cannot be used as a quantitative
metric for aerosol size integrated through the column <xref ref-type="bibr" rid="bib1.bibx50 bib1.bibx34" id="paren.46"/>. Instead, we interpret <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> results as being qualitatively
indicative of the aerosol type present in the column – either fine (values
close to 2) or coarse (values between 0 and 1). Due to the qualitative nature
of the variable, combined with the fact that <inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">α</mml:mi><mml:mrow><mml:mn>550</mml:mn><mml:mo>/</mml:mo><mml:mn>865</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> and
<inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">α</mml:mi><mml:mrow><mml:mn>470</mml:mn><mml:mo>/</mml:mo><mml:mn>660</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> are highly correlated (<inline-formula><mml:math display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mi mathvariant="italic">&gt;</mml:mi><mml:mn>0.8</mml:mn></mml:mrow></mml:math></inline-formula>) at all sites, we will
refer to <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> without specifying wavelength.</p>
      <p>Considering Fig. <xref ref-type="fig" rid="Ch1.F6"/>, <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> shows trends similar to AOD
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>). Generally there is a maximum in <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> of 1.0–1.8
during spring and through summer, gradually decreasing through fall to reach
a minimum of 0.6–1.0 during winter. This suggests that fine particles are
most abundant in the column in spring when biomass burning impacts South
Africa, agreeing with previous results suggesting that aerosol plumes
transported to South Africa tend to be characterized by mainly Aitken mode
(0.01–0.1 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) aerosol <xref ref-type="bibr" rid="bib1.bibx37 bib1.bibx17 bib1.bibx22 bib1.bibx49" id="paren.47"/>. <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> remains high through the hot, photochemically intense
summer months, when significant fine, secondary sulfate, nitrate, and organic
aerosol is produced from abundant industrial emissions of SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>,
NO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula>, and volatile organic compounds (VOCs), respectively <xref ref-type="bibr" rid="bib1.bibx37 bib1.bibx45 bib1.bibx26" id="paren.48"/>, and when as many as 86 % of days in industrial areas display
new particle formation <xref ref-type="bibr" rid="bib1.bibx26" id="paren.49"/>. This is in contrast to the dry
winter months, when <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> is low and it appears as though particles above
the major metropolitan areas of South Africa tend to be larger – suggesting
a greater contribution from dust or large soot particles. <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> is
relatively constant throughout the year in Cape Town, indicative of a
consistent aerosol size distribution resulting from clean, marine air-mass
origin and fairly constant local generation of marine aerosol. At the other
coastal site (Durban), <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> is similarly high throughout the year, but
displays a strong seasonal biomass burning signal in spring owing to its
location near major sources of small biomass burning particles in local
sugar cane fields and in Zimbabwe and Mozambique.</p>
      <p>In addition to a clear impact on <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> by transported biomass burning
emissions, maxima and minima in <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> are highly correlated with CWV in
all regions except Cape Town (Fig. <xref ref-type="fig" rid="Ch1.F5"/>; <inline-formula><mml:math display="inline"><mml:mrow><mml:mn>0.64</mml:mn><mml:mi mathvariant="italic">&lt;</mml:mi><mml:mi>r</mml:mi><mml:mi mathvariant="italic">&lt;</mml:mi><mml:mn>0.98</mml:mn></mml:mrow></mml:math></inline-formula>).
This result agrees with Kumar et al. (<xref ref-type="bibr" rid="bib1.bibx32" id="year.50"/>), who found that
CWV correlated well with <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>, but not AOD. The relationship between CWV
and <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> is unlikely to be causal, but rather coincidental since wet
summer months tend to have suppressed dust generation (fewer large particles and
higher <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>) and enhanced secondary photochemical aerosol production
(more small particles and higher <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>). Overall, <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> for inland
sites (Bloemfontein, Gauteng, HVAPA) is significantly lower on average than
for coastal sites (Cape Town and Durban), with <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="italic">α</mml:mi><mml:mi mathvariant="italic">&lt;</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> for much of the
year. This supports previous findings that coarse particles such as dust form
an important contribution to column aerosol loading, and appear to dominate
the aerosol size distribution at inland sites <xref ref-type="bibr" rid="bib1.bibx37 bib1.bibx45 bib1.bibx26" id="paren.51"/>.</p>
      <p>Values of <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> reported here are lower than previously reported in
Southern Africa, primarily because major studies of aerosol optical
properties in the region have focused on intensive periods of biomass
burning. Eck et al. (<xref ref-type="bibr" rid="bib1.bibx17" id="year.52"/>) found high <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> near biomass
burning sources in Zambia (1.8–1.9) during biomass burning season from
August-October, while Robles-Gonzalez, et al. (<xref ref-type="bibr" rid="bib1.bibx52" id="year.53"/>) measured <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> as high as 2.1 in burning
regions. Kumar et al. (<xref ref-type="bibr" rid="bib1.bibx32" id="year.54"/>) found strong seasonal
variability at a site in northeastern South Africa, with high <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> (up to
2.9) during burning season, but much lower <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> (0.5) during the rest of
the year. Ranges of <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> similar to those reported here have been
observed in urban and industrial sites in China (ranging from 0.5–1.6 in Qi
et al. (<xref ref-type="bibr" rid="bib1.bibx47" id="year.55"/>), with an annual average of 1.25 in Zhuang et al. (<xref ref-type="bibr" rid="bib1.bibx69" id="year.56"/>).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7"><caption><p>Monthly averaged values of UVAI for each region for the period 1 January 2000 to 31 December 2009.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f07.pdf"/>

          </fig>

</sec>
<sec id="Ch1.S3.SS2.SSS3">
  <title>Ultraviolet Aerosol Index (UVAI)</title>
      <p>Month averages of Ultraviolet Aerosol Index (UVAI) from the Total Ozone
Mapping Spectrometer (TOMS) are presented for each region in Fig. <xref ref-type="fig" rid="Ch1.F7"/>. UVAI is a qualitative metric based on the difference between
the ratio of absorbing and non-absorbing spectral radiance ratios provided by
satellite observations and model calculations. High values of UVAI are
associated with high concentrations of strongly absorbing aerosols – namely
UV-absorbing soot, smoke, and mineral dust <xref ref-type="bibr" rid="bib1.bibx27" id="paren.57"/>, as well as ash
and brown carbon. UVAI reaches a maximum of 1.0–1.2 in spring and remains
high through summer before decreasing to a minimum of 0.7 during winter. This
trend highlights the influence of strongly absorbing biomass burning and dust
aerosol, which are most prevalent through spring. Trends in UVAI generally
follow those of AOD (Fig. <xref ref-type="fig" rid="Ch1.F2"/>) and exhibit good correlation with
MISR AOD (<inline-formula><mml:math display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>∼</mml:mo><mml:mn>0.6</mml:mn></mml:mrow></mml:math></inline-formula>), except for the Cape Town region where marine
aerosol appears to dictate column aerosol properties. The only statistically
significant difference between sites is observed in Durban during August and
September, when UVAI is elevated relative to other sites owing to significant
emissions of strongly absorbing biomass burning emissions from local sugar
cane burning <xref ref-type="bibr" rid="bib1.bibx33" id="paren.58"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8"><caption><p>Monthly averaged fractional contribution of various aerosol components to total
AOD as modeled by GOCART. Data are presented for each region for the period 1 January 2000 to 31 December 2009.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f08.pdf"/>

          </fig>

</sec>
<sec id="Ch1.S3.SS2.SSS4">
  <title>Goddard Ozone Chemistry Aerosol Radiation and Transport (GOCART) model</title>
      <p>GOCART model results estimate the contribution of dust, black carbon, organic
carbon, sulfate, and sea salt to total column AOD, based on global emissions
inventories <xref ref-type="bibr" rid="bib1.bibx10" id="paren.59"/>. Total estimated GOCART AOD is presented in
Fig. <xref ref-type="fig" rid="Ch1.F2"/>, and the fraction of AOD attributed to each modeled
constituent is displayed in Fig. <xref ref-type="fig" rid="Ch1.F8"/>. The monthly averaged
fractional contribution of each aerosol component is very consistent across
sites, displaying high <inline-formula><mml:math display="inline"><mml:mi>r</mml:mi></mml:math></inline-formula> for individual components (i.e., dust in Johannesburg
compared with dust in Durban for a particular month); typically <inline-formula><mml:math display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 0.9. Only Cape Town exhibits a unique trend, owing largely to the
significantly larger modeled contribution of dust throughout the year.
Modeled dust enhancement in Cape Town is especially pronounced from May
through July, when emissions inventories include a large contribution from
windblown dust from the nearby Namib Desert. Such an enhancement in the
contribution of dust would presumably result in an enhancement in UVAI during
May–July and a general trend of elevated UVAI in Cape Town, which is not
observed in the data. Further, GOCART results do not capture the enhancement
in dust aerosol expected in late winter to early spring (JAS) based on AOD,
UVAI, and enhanced ground wind speed in dry conditions. We therefore suggest
that GOCART emissions inventories either significantly overestimate dust in
Cape Town or underestimate dust emissions for the rest of South Africa. Given
the consistent UVAI across sites in Fig. <xref ref-type="fig" rid="Ch1.F7"/>, the strong potential
for dust generation in early spring when winds increase but before
precipitation arrives, and previous work indicating that <inline-formula><mml:math display="inline"><mml:mrow><mml:mi mathvariant="italic">&gt;</mml:mi><mml:mn>70</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="italic">%</mml:mi></mml:mrow></mml:math></inline-formula> of coarse
and &gt; 40 % of fine particle mass is contributed by dust at sites in the
Eastern Cape and Highveld <xref ref-type="bibr" rid="bib1.bibx45 bib1.bibx46" id="paren.60"/>, we suggest that
GOCART significantly underestimates dust as an aerosol source over the
majority of South Africa.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9"><caption><p>Frequency of air-mass origin based on seasonal averages (summer: DJF, fall:
MAM, winter: JJA, spring: SON) of 3-day HYSPLIT back-trajectories for Gauteng for
the period 1 January 2000 to 31 December 2009. Colors correspond to percentage
frequency with which air mass arriving in Gauteng originates at a particular location within the previous 3 days.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f09.pdf"/>

          </fig>

</sec>
</sec>
<sec id="Ch1.S3.SS3">
  <title>Ground-based sampling results</title>
      <p>Ground-based air quality data were obtained through monitoring networks
within the Gauteng satellite grid box comprising the cities of Johannesburg
and Tshwane (Pretoria), as well as the Ekurhuleni Metro Area (east of the City of
Johannesburg) and the Vaal Triangle AQ Priority Area (VTAPA). Table <xref ref-type="table" rid="Ch1.T1"/> summarizes data type and date ranges available for
sites utilized in this study. Sites were classified as one of four types:
township or informal settlement sites characterized by some domestic burning
emissions (Township/Domestic Burning), developed residential areas in either
urban or suburban settings with no domestic burning emissions (Urban/Suburban
Residential), areas rich with industrial or power generation activities
(Industrial), or sites aimed at capturing on-road sources (Traffic). An
emissions summary for the Gauteng area (Fig. <xref ref-type="fig" rid="Ch1.F1"/>) indicates
that the most significant area sources are from biomass burning (veld fires
that occur in early to mid-winter), informal settlements (primarily domestic
burning throughout the winter), and mine tailings and waste dumps (emissions
dependent on wind speed). The most significant point sources in Gauteng are
three coal-fired power plants and two petrochemical refineries in the south,
and five steel manufacturing facilities and three cement manufacturing
facilities to the south and central part of the region.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F10"><caption><p>Monthly averaged PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula>, PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> (absolute magnitude and normalized
by maximum monthly average) and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula>/PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> for ground monitoring sites.
Solid lines represent sites with domestic burning influence, fine dashed lines
represent urban/suburban residential areas, and coarse dashed lines represent industrial sites.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f10.pdf"/>

        </fig>

      <p><?xmltex \hack{\newpage}?>Seasonally averaged HYSPLIT back-trajectory frequencies (Fig. <xref ref-type="fig" rid="Ch1.F9"/>) indicate typical air-mass origin for Gauteng. Summer and
fall are characterized by air arriving from the east and southeast, while
winter is directionally distributed and spring typically sees air transported
from the north and east (Zimbabwe and Mozambique), with some contribution
from the southwest and southeast. Local meteorology for Gauteng (Fig. <xref ref-type="fig" rid="Ch1.F4"/>) was described above and is characterized by cool and
very dry winters, with temperature and precipitation increasing through the
spring to maxima in the summer. Wind speed increases before precipitation in
the spring, resulting in local dust generation from July through September.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F11" specific-use="star"><caption><p>Season-averaged diurnal PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula>, with each site normalized
by the maximum hourly average across all seasons. Solid lines represent sites with
domestic burning influence, fine dashed lines represent urban/suburban
residential areas, and coarse dashed lines represent industrial sites.</p></caption>
          <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f11.pdf"/>

        </fig>

      <p>Monthly averages of PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula>, both in absolute magnitude and
normalized by each site's maximum monthly average, are presented in Fig. <xref ref-type="fig" rid="Ch1.F10"/>. PM concentrations reach a maximum during winter (June,
July, and August) for all except industrial sites. This maximum in PM
concentrations corresponds to the coldest months, when the most significant
domestic burning activity is expected and boundary layers are extremely
shallow (often 50 m or less). The summer maximum in industrial areas may
result from photochemistry of industrial precursors and generation of
secondary particulates, or may be due to atmospheric dynamics. During winter,
industrial stack emissions tend to be released far above the very shallow
boundary layer and into a stable atmosphere. During summer, on the other hand,
deeper boundary layers extend above stacks and industrial emissions therefore
stay within a less stable boundary layer, resulting in mixing of emissions
to the ground. The average monthly ratio of PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> to PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> was
calculated for sites with both parameters, and there is no statistically
significant monthly variability. This suggests that fine particles comprise a
relatively consistent fraction of total particulate concentration throughout
the year, despite large changes in overall particulate concentration.</p>
      <p>Diurnal averages of PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> for each season are presented in
Fig. <xref ref-type="fig" rid="Ch1.F11"/>. PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations
have been normalized by the maximum hourly average for each site for the
entire year (typically between 19:00 and 21:00 LT during winter), with the
average concentration (in absolute magnitude) for each type of site displayed
in the third row of diurnal plots. As was evident in monthly PM data, the
highest concentrations occur in township areas where domestic burning is
expected, followed by significantly lower PM concentrations in urban and
suburban residential areas and the lowest concentrations on average in
industrial areas. The clearest feature in the diurnal data is the significant
enhancement in particulate concentrations in the morning (06:00–09:00 LT) and
evening (17:00–22:00 LT) during all seasons. This trend is especially
dramatic during winter, with typical evening PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula>
concentration maxima in township areas of 203 and 105 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math 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>,
respectively, with evening PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> maxima averaging in excess of 400 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math 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 some sites.</p>
      <p>That these diurnal patterns of enhanced PM concentration in morning and
evening are discernible in all seasons is evidence that domestic burning
impacts air quality in South Africa throughout the year. The significant
enhancement in PM during winter underscores the fact that increased burning
during cold months within shallow boundary layers consistently leads to
dangerous concentrations of particulates – particularly in the lowest-income
residential areas. It should be mentioned that the observed diurnal patterns
may also reflect some contribution from on-road emissions – either primary
combustion or vehicle-associated dust particles. However, the high density of
domestic burning and relatively low density of vehicles in townships compared
with other areas suggests that these on-road sources should be minor compared
with primary burning emissions. The diurnal ratio of PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> to PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula>
is displayed in Fig. <xref ref-type="fig" rid="Ch1.F12"/>, and reaches a maximum at all
township sites during burning periods, indicating that morning and evening
domestic burning activity tends to be a source of small particles.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F12" specific-use="star"><caption><p>Season-averaged diurnal PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula>/PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula>, indicating the diurnal
variability in the ratio of fine to coarse particles. Solid lines represent
sites with domestic burning influence, fine dashed lines represent urban/suburban
residential areas, and coarse dashed lines represent industrial sites.</p></caption>
          <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f12.pdf"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F13" specific-use="star"><caption><p>Average diurnal PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> for each site type.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f13.pdf"/>

        </fig>

      <p>Average diurnal profiles for each site type are presented in Fig. <xref ref-type="fig" rid="Ch1.F13"/>, and diurnal and monthly maxima, minima, and mean
values for both PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> are presented in Table <xref ref-type="table" rid="Ch1.T3"/>. On average, PM concentrations in townships are 51 %
higher than urban/suburban residential sites and 78 % higher than industrial
sites, underscoring the importance of domestic emissions as associated with
the highest concentrations of particles in the region. The difference between
townships and other areas is more distinct in winter, when PM concentrations
in townships are 63 and 135 % higher than in urban/suburban residential and
industrial sites, respectively. The average wintertime evening maximum in
PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> at townships is 203 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math 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 average 1-h concentrations
approaching 400 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math 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 many township sites. PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> concentrations
are markedly higher than PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> during burning periods, indicating that
while domestic burning tends to enhance small particles (above), much of the particulate mass is
still associated with large particles (&gt; 2.5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m). This agrees
with results from Wentzel et al. (<xref ref-type="bibr" rid="bib1.bibx64" id="year.61"/>), who found giant
dendritic carbonaceous aerosols associated with burning at a township site in
Gauteng. There is significant variability in PM concentrations between sites
just a few kilometers apart, indicating that the domestic burning that
generates the highest concentrations of particulates is highly localized and
most dramatically impacts air quality in a small area in the immediate
vicinity of emissions. This result indicates that domestic burning PM source
strength in low-income areas is highly variable, depending on factors such as
the availability of electricity, the method of burning coal or wood, and
thermal efficiency of homes.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T3" specific-use="star"><caption><p>Average diurnal and monthly values of PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> measured at the ground, separated by site type. All concentrations in <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math 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></caption><oasis:table frame="topbot"><oasis:tgroup cols="6">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:colspec colnum="5" colname="col5" align="left"/>
     <oasis:colspec colnum="6" colname="col6" align="left"/>
     <oasis:thead>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3"/>  
         <oasis:entry colname="col4">Township</oasis:entry>  
         <oasis:entry colname="col5">Urban/Suburban</oasis:entry>  
         <oasis:entry colname="col6">Industrial</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3"/>  
         <oasis:entry colname="col4"/>  
         <oasis:entry colname="col5">Residential</oasis:entry>  
         <oasis:entry colname="col6"/>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2">Diurnal</oasis:entry>  
         <oasis:entry colname="col3">Max</oasis:entry>  
         <oasis:entry colname="col4">408</oasis:entry>  
         <oasis:entry colname="col5">130</oasis:entry>  
         <oasis:entry colname="col6">162</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Min</oasis:entry>  
         <oasis:entry colname="col4">14</oasis:entry>  
         <oasis:entry colname="col5">8</oasis:entry>  
         <oasis:entry colname="col6">7</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">Monthly</oasis:entry>  
         <oasis:entry colname="col3">Max</oasis:entry>  
         <oasis:entry colname="col4">169</oasis:entry>  
         <oasis:entry colname="col5">88</oasis:entry>  
         <oasis:entry colname="col6">109</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Min</oasis:entry>  
         <oasis:entry colname="col4">23</oasis:entry>  
         <oasis:entry colname="col5">28</oasis:entry>  
         <oasis:entry colname="col6">10</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Mean</oasis:entry>  
         <oasis:entry colname="col4">70 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 31</oasis:entry>  
         <oasis:entry colname="col5">46 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 16</oasis:entry>  
         <oasis:entry colname="col6">39 <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 23</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2">Diurnal</oasis:entry>  
         <oasis:entry colname="col3">Max</oasis:entry>  
         <oasis:entry colname="col4">123</oasis:entry>  
         <oasis:entry colname="col5"/>  
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Min</oasis:entry>  
         <oasis:entry colname="col4">12</oasis:entry>  
         <oasis:entry colname="col5"/>  
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2">Monthly</oasis:entry>  
         <oasis:entry colname="col3">Max</oasis:entry>  
         <oasis:entry colname="col4">72</oasis:entry>  
         <oasis:entry colname="col5"/>  
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Min</oasis:entry>  
         <oasis:entry colname="col4">23</oasis:entry>  
         <oasis:entry colname="col5"/>  
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"/>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3">Mean</oasis:entry>  
         <oasis:entry colname="col4">38<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 12</oasis:entry>  
         <oasis:entry colname="col5"/>  
         <oasis:entry colname="col6"/>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p>Data from two township sites (Alexandra and Bodibeng) have diurnal trends
that do not conform to the typical morning and evening PM enhancements
typical of low-income areas, and represent intriguing qualitative case
studies in the impact of township evolution and informal commercial activity
within the township context. Both townships are well-developed, and
electricity is the primary fuel used for heating and cooking in households.
Qualitatively speaking (data are not available), both townships have a high
density of informal food vendors that cook almost exclusively over open
flames using inefficient three-stone fires which emit large concentrations of
particulates <xref ref-type="bibr" rid="bib1.bibx5" id="paren.62"/>. Vendors start cooking in the early morning
and continue throughout the day and into the evening, which may be the source
of the diurnal PM profile which does display moderate concentration
enhancements in morning and (more pronounced) evening but also displays elevated PM
concentrations at midday.</p>
</sec>
<sec id="Ch1.S3.SS4">
  <title>Satellite data as a proxy for air quality</title>
      <p>As discussed above, while there is a trend of using remotely sensed data as a
proxy for air quality at the ground, it is necessary to evaluate the
appropriateness of this practice in each individual area. Figure <xref ref-type="fig" rid="Ch1.F14"/> displays month-averaged PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula>
concentrations from ground monitoring sites throughout Gauteng, plotted
against month-averaged satellite parameters (AOD, <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> and UVAI) for the
Gauteng satellite grid box. Solid lines represent least-squares linear
regression fits, considered separately for each ground monitoring site type.
<inline-formula><mml:math display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> values for linear regressions are annotated on the figure. Poor
correlation is immediately evident between PM concentrations and both AOD and
UVAI, and indeed none of the relationships are statistically significant.
Further, what correlation does exist is the opposite of what is expected –
since AOD and UVAI both capture overall light extinction due to particles,
one would expect elevated PM concentration to correspond with elevated AOD
and UVAI. However, the highest PM concentrations occur at the ground during
winter months, when AOD and UVAI are at a minimum, while the maxima in AOD
and UVAI tend to occur during spring and into the summer, when deeper
boundary layers and an absence of domestic burning result PM concentration
minima. The correlations between PM concentration and <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> are
statistically significant (except in industrial areas), with low <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>
(larger particles in the column) corresponding to higher concentrations at
the ground. We suggest that this correlation is coincidental.
High PM concentrations at the ground correspond to domestic burning and
occur during winter, when large dust particles appear to be more prevalent
in the column (low <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>). To our knowledge, this is the first published study to report
such generalized disagreement between remotely sensed aerosol properties and
PM concentrations at the ground.</p>
      <p>There are a number of reasons for the discrepancy between ground and
satellite data in metropolitan areas of South Africa. First, and most
important, there is strong potential for vertical inhomogeneity to result in
a disconnect between column and ground aerosol properties in the region. For example,
Campbell et al. (<xref ref-type="bibr" rid="bib1.bibx6" id="year.63"/>) and Chand et al. (<xref ref-type="bibr" rid="bib1.bibx9" id="year.64"/>) indicated that biomass burning emissions from fires
in the tropics tend to be transported to South Africa in stratified layers
aloft, and Tyson et al. (<xref ref-type="bibr" rid="bib1.bibx62" id="year.65"/>) found that there are
frequent, persistent, absolutely stable layers at 3 and 5 km above much of
South Africa, increasing the potential for stratified plumes of pollutants
above the ground. While concentrated plumes of particles in stratified layers
above the ground would impact column aerosol properties, they would not
affect ground concentrations of particulates unless atmospheric instability
caused those particles to be vertically mixed into the planetary boundary
layer and to the surface. Therefore, characteristics of column aerosol
properties are not necessarily indicative of any trends in ground PM
concentrations – particularly in South Africa's stratified atmosphere.</p>
      <p>Next, the highest concentrations of particulates in South Africa are observed
during winter, when domestic burning emissions are released into an extremely
shallow boundary layer – often on the order of 50 m or less
<xref ref-type="bibr" rid="bib1.bibx62" id="paren.66"/>. Because these emissions are confined in a layer so close
to the ground, it is unlikely that satellite retrievals are able to resolve
the difference between the concentrated aerosol layer and the ground itself.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F14" specific-use="star"><caption><p>Monthly averaged PM for each site type (domestic burning, urban/suburban
residential, and industrial) plotted against monthly averaged satellite parameters
(AOD, <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>, and UVAI). Linear least squares regression lines are plotted,
with corresponding <inline-formula><mml:math display="inline"><mml:mrow><mml:msup><mml:mi>R</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> values listed for each fit.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f14.pdf"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F15"><caption><p>Winter diurnal ground PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations, with shaded
gray boxes representing satellite flyover times for MODIS-Terra, MODIS-Aqua, and MISR platforms.</p></caption>
          <?xmltex \igopts{width=199.169291pt}?><graphic xlink:href="https://www.atmos-chem-phys.net/15/4259/2015/acp-15-4259-2015-f15.pdf"/>

        </fig>

      <p>Third is the issue of temporal resolution. Figure <xref ref-type="fig" rid="Ch1.F15"/> shows
average wintertime PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> diurnal profiles for each site
type, with shaded boxes representing the time window in which MODIS-Terra,
MISR, and MODIS-Aqua instruments pass over South Africa. MODIS-Terra and MISR
(09:00 to 11:00 LT) tend to pass over South Africa on the tail end of
enhanced PM concentrations from morning domestic burning, while Aqua's pass
over time (13:00–15:00 LT) coincides with the minimum PM concentrations of
the day. While PM concentrations tend to be elevated throughout the day at
all sites during winter, the average daily, weekly, and winter PM
concentrations at the ground are strongly influenced by morning and evening
maxima that are not observed by satellites. Therefore, the discrepancy
between satellite passover times and elevated PM concentrations indicates
that remotely sensed data are unlikely to capture the trend of significantly
enhanced PM concentration at the ground.</p>
      <p>Finally, spatial resolution may be a factor prohibiting satellite data from
appropriately representing ground PM concentrations. PM concentrations
between township, suburban, and industrial sites just a few km apart are
significantly different (Fig. <xref ref-type="fig" rid="Ch1.F10"/>), underscoring the
significant local variability in PM concentrations resulting from unique
source density in each area. Satellite measures of aerosol properties must be
averaged over spatial scales on the order of 1 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>, which
includes many areas with low overall concentrations and areas (e.g.,
urban/suburban residential and industrial in Fig. <xref ref-type="fig" rid="Ch1.F13"/>)
where the discrepancy between seasonal profiles of PM do not vary
significantly in magnitude. These highly localized gradients in PM at the
ground occur on scales much smaller than the resolution of level 2 or level 3 data
available from MODIS-Aqua and MODIS-Terra, and indeed level 2 data display no
better correlation than the level 3 data presented in this work.</p>
      <p>Overall, the problem of extreme PM concentrations at the ground appears to be
a highly localized one impacting primarily low-income areas of South Africa,
and the vertical integration, low time resolution, and spatial averaging
required with satellite data precludes their use in understanding and
predicting ground PM characteristics in the South African context.</p>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <title>Conclusions</title>
      <p>Here we present a comprehensive study of
air quality in South Africa's metropolitan centers, based on decadal averages
of remotely sensed aerosol column data and multi-year averages from
ground-based air quality sampling sites. Aerosol climatology from satellite
platforms was based on AOD, Ångström exponent and UVAI, and GOCART
model results were also analyzed. AOD was found to reach a maximum of
0.12–0.20 during late winter and early spring (ASO), corresponding with elevated
column concentrations of absorbing aerosol from close-proximity fires in
Mozambique, Zimbabwe, and eastern South Africa, as well as from enhanced
windblown dust generation during dry and windy months. Minimum AOD of
0.05–0.10 occurs during winter, when domestic burning emissions are highest
and air quality at the ground is worst, suggesting that this aerosol is
confined to a very shallow layer and does not impact overall column aerosol
characteristics despite its importance at the surface. AOD in metropolitan
areas of South Africa is a factor of 3–6 lower than reported for megacities
worldwide, and is lower than previously reported in the rural northeast part
of the country that is closer in proximity to biomass burning sources.
Ångström exponent reaches a maximum of 1.0–1.8 during spring and summer
at sites closest to biomass burning sources, reflecting the importance of
regional fires as sources of small particles. Ångström reaches a
minimum of 0.6–1.0 in winter, when dry conditions appear to result in an
enhanced contribution of coarse dust particles to column aerosol.
Ångström exponent is highly correlated with CWV and is markedly lower
at continental sites, suggesting that coarse dust particles contribute
significantly to total column aerosol in inland South Africa. UVAI reaches a
maximum of 1.0–1.2 during spring and summer, coinciding with the presence of
strongly absorbing dust and biomass burning particles. UVAI reaches a minimum of
0.7 in winter, when dust aerosols appear to contribute a larger fraction of
column aerosol but integrated column concentrations are very low. Satellite
results in Cape Town are significantly different than other sites, reflecting
a difference between clean marine versus polluted continental air-mass
origins. Overall, satellite data provide a good representation of
large-scale, regional, and seasonal trends in column particulates across
South Africa.</p>
      <p>Ground air quality results are based on PM data from 19 sites in Gauteng
province, which is the most significant population and industrial center of
South Africa. Ground monitoring sites fall into 4 categories: township areas
with close proximity domestic burning, urban/suburban residential areas,
industrial areas, and traffic sites directly adjacent to major on-road
sources. Based on monthly averages, townships experience 51 and 78 % higher
PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> concentrations than urban/suburban residential and industrial
areas, respectively. This quantitatively confirms previous studies indicating
that the poorest air quality in South Africa is found in low-income areas
<xref ref-type="bibr" rid="bib1.bibx18 bib1.bibx19 bib1.bibx20 bib1.bibx23 bib1.bibx44" id="paren.67"><named-content content-type="pre">e.g.,</named-content></xref>. Both PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> reach distinct maxima during winter
(June, July, or August) in all non-industrial sites, while two maxima are
observed in industrial sites and correspond to photochemical particulate
production and deeper, unstable boundary layers in summer and domestic
burning in winter. Both PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> display diurnal patterns at
all sites, with elevated concentration in the morning (06:00–09:00 LT) and
maximum concentration in the evening (17:00–22:00 LT) in all seasons. These
diurnal profiles are especially distinct during winter in low-income areas,
with evening PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> 1 h average mass concentrations
reaching 203 and 105 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>g m<inline-formula><mml:math 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>, respectively. Monthly and diurnal PM
concentrations at the ground vary significantly between sites just a few km
apart, underscoring the importance of source strength and density in
determining particulate air quality at a highly localized level. This result
also indicates that a “typical” low income area is difficult to define solely
in terms of the magnitude of particulate concentration.</p>
      <p>If satellite measurements of column aerosol properties were an appropriate
proxy for air quality at the ground in urban South Africa, one would expect
AOD to be positively correlated with PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations.
This, however, is not observed, as correlations between AOD and PM are weak
and negative. PM<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn>10</mml:mn></mml:msub></mml:math></inline-formula> is negatively correlated with <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula>, suggesting
that higher ground PM concentrations are associated with larger particles in
the column. We suggest, however, that this correlation is coincidental due to
seasonal variation in which high wintertime PM concentrations at the ground
occur during the dry season when coarse dust particles contribute an elevated
fraction of column aerosol. Other satellite and model products show little
correlation with ground PM concentrations, and it appears as though
satellites are unable to resolve even extremely high PM concentrations at the
ground during winter in South Africa. This discrepancy is likely the result
of a combination of atmospheric dynamics (absolutely stable layers aloft,
concentrated pollutants transported aloft, and high wintertime PM confined
within a very shallow boundary layer) and time and spatial resolution
(satellites pass over southern Africa during off-peak times for PM
concentration, and data must be averaged over large areas).</p>
      <p>The inability of satellites to capture trends in ground PM concentrations in
South Africa indicates that monitoring and characterization of air quality in
South Africa will require extensive networks of ground monitoring stations
producing quality data across the country, as well as intensive
multi-platform campaigns aimed at understanding the relationship between
ground and remotely sensed air quality data. Further advances in
understanding would follow regular monitoring of vertical profiles of
criteria pollutants. South Africa's current monitoring networks are in
varying states of functionality and management, meaning that many air quality
data time series are either incomplete or poor in quality. Data are
controlled individually by each network, so a study like this one requires
many different official requests, approvals, and waiting times for data.
Further, these monitoring sites tend to be in urban and industrial centers of
South Africa like those considered in this work. However, roughly 40 % of
South Africa's population resides in rural settlements, and little is known
about air quality in these areas. Based on results presented here, we suggest
that a systematic effort be made in South Africa to improve and centralize
management, data quality, and data availability amongst existing ground
monitoring networks, in addition to an expansion of ground monitoring sites
into rural areas.</p>
</sec>

      
      </body>
    <back><ack><title>Acknowledgements</title><p>The authors would like to acknowledge the South African Weather Service
(SAWS) for providing meteorology data from ground monitoring sites and for
coordinating ground data from air quality monitoring stations. The authors
would also like to thank the air quality monitoring networks in Johannesburg,
Tshwane, Ekurhuleni, and the Vaal Triangle Priority Area reporting to SAAQIS.
Armin Sorooshian, Ewan Crosbie, and Taylor Schingler acknowledge support in
part by Grant 2 P42 ES0494011 from the National Institute of Environmental
Health Sciences (NIEHS) Superfund Research Program, NIH, and the Center for
Environmentally Sustainable Mining through TRIF Water Sustainability Program
funding. Rebecca M. Garland acknowledges support of a grant from CSIR. This
work is based on the research supported in part by the National Research
Foundation of South Africa (grant number 81659) to Stuart Piketh.<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>
Edited by: P. Formenti</p></ack><ref-list>
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