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

    <article-meta>
      <article-id pub-id-type="doi">10.5194/acp-16-8181-2016</article-id><title-group><article-title>Retrieval of aerosol optical depth from surface solar radiation measurements
using machine learning algorithms, non-linear regression and a radiative
transfer-based look-up table</article-title>
      </title-group><?xmltex \runningtitle{Retrieval of aerosol optical depth from surface solar radiation measurements}?><?xmltex \runningauthor{J. Huttunen et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Huttunen</surname><given-names>Jani</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Kokkola</surname><given-names>Harri</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1404-6670</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Mielonen</surname><given-names>Tero</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Mononen</surname><given-names>Mika Esa Juhani</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Lipponen</surname><given-names>Antti</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-6902-9974</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Reunanen</surname><given-names>Juha</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Lindfors</surname><given-names>Anders Vilhelm</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-9305-0864</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Mikkonen</surname><given-names>Santtu</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-0595-0657</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff2">
          <name><surname>Lehtinen</surname><given-names>Kari Erkki Juhani</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5 aff6">
          <name><surname>Kouremeti</surname><given-names>Natalia</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff6">
          <name><surname>Bais</surname><given-names>Alkiviadis</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-3899-2001</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Niska</surname><given-names>Harri</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Arola</surname><given-names>Antti</given-names></name>
          <email>antti.arola@fmi.fi</email>
        </contrib>
        <aff id="aff1"><label>1</label><institution>Finnish Meteorological Institute (FMI), Atmospheric
Research Centre of Eastern Finland, Kuopio, Finland</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Department of Applied Physics, University of Eastern
Finland, Kuopio, Finland</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Independent researcher, Kuopio, Finland</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Tomaattinen Oy, Helsinki, Finland</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>Physikalisch-Meteorologisches Observatorium Davos,
Dorfstrasse 33, 7260 Davos Dorf, Switzerland</institution>
        </aff>
        <aff id="aff6"><label>6</label><institution>Aristotle University of Thessaloniki, Laboratory of
Atmospheric Physics, Thessaloniki, 54124, Greece</institution>
        </aff>
        <aff id="aff7"><label>7</label><institution>Department of Environmental and Biological Sciences,
University of Eastern Finland, Kuopio, Finland</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Antti Arola (antti.arola@fmi.fi)</corresp></author-notes><pub-date><day>7</day><month>July</month><year>2016</year></pub-date>
      
      <volume>16</volume>
      <issue>13</issue>
      <fpage>8181</fpage><lpage>8191</lpage>
      <history>
        <date date-type="received"><day>20</day><month>January</month><year>2016</year></date>
           <date date-type="rev-request"><day>25</day><month>January</month><year>2016</year></date>
           <date date-type="rev-recd"><day>9</day><month>June</month><year>2016</year></date>
           <date date-type="accepted"><day>14</day><month>June</month><year>2016</year></date>
      </history>
      <permissions>
<license license-type="open-access">
<license-p>This work is licensed under a Creative Commons Attribution 3.0 Unported License. To view a copy of this license, visit <ext-link ext-link-type="uri" xlink:href="http://creativecommons.org/licenses/by/3.0/">http://creativecommons.org/licenses/by/3.0/</ext-link></license-p>
</license>
</permissions><self-uri xlink:href="https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016.html">This article is available from https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016.html</self-uri>
<self-uri xlink:href="https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016.pdf</self-uri>


      <abstract>
    <p>In order to have a good estimate of the current forcing by anthropogenic
aerosols, knowledge on past aerosol levels is needed. Aerosol optical depth
(AOD) is a good measure for aerosol loading. However, dedicated measurements
of AOD are only available from the 1990s onward. One option to lengthen the AOD
time series beyond the 1990s is to retrieve AOD from surface solar radiation
(SSR) measurements taken with pyranometers. In this work, we have evaluated
several inversion methods designed for this task. We compared a look-up
table method based on radiative transfer modelling, a non-linear regression
method and four machine learning methods (Gaussian process, neural network,
random forest and support vector machine) with AOD observations carried out with a
sun photometer at an Aerosol Robotic Network (AERONET) site in Thessaloniki,
Greece. Our results show that most of the machine learning methods produce
AOD estimates comparable to the look-up table and non-linear regression
methods. All of the applied methods produced AOD values that corresponded
well to the AERONET observations with the lowest correlation coefficient
value being 0.87 for the random forest method. While many of the methods
tended to slightly overestimate low AODs and underestimate high AODs, neural network and support vector machine showed overall better correspondence for
the whole AOD range. The differences in producing both ends of the AOD range
seem to be caused by differences in the aerosol composition. High AODs were
in most cases those with high water vapour content which might affect the
aerosol single scattering albedo (SSA) through uptake of water into
aerosols. Our study indicates that machine learning methods benefit from the
fact that they do not constrain the aerosol SSA in the retrieval, whereas
the LUT method assumes a constant value for it. This would also mean that
machine learning methods could have potential in reproducing AOD from SSR
even though SSA would have changed during the observation period.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p>The Fifth Assessment Report of the Intergovernmental Panel on Climate Change
states that the most significant source of uncertainty in the projections of
climate is related to aerosols (IPCC, 2013). One significant contribution to
this uncertainty comes from the fact that without the knowledge of the
aerosol burden in the past, we are not able to estimate the current forcing
of anthropogenic aerosol. For example, the effect of changes in the current
aerosol emissions on climate depends on the background aerosol load during
the pre-industrial era (e.g. Andreae and Rosenfeld, 2008; Carslaw et al., 2013). In
addition, the current estimates of past aerosol emissions are highly
uncertain (Granier et al., 2011), thus increased knowledge on historical
aerosol levels would increase our ability to estimate the present day
aerosol radiative forcing.</p>
      <p>One limiting factor in determining the properties of global aerosol in the
past has been that observations of aerosol radiative effects have been
limited to fairly recent periods. For example, the aerosol optical depth has
mainly been measured using sun photometers and the most widely known
ground-based network of sun photometers is Aerosol Robotic Network (AERONET;
Holben et al., 1998). Although, AERONET already contains over
700 stations globally, with a fairly good spatial coverage compared to many other
observation networks, it still lacks in temporal coverage, having provided aerosol
optical properties and AOD only since 1990s and reaching the current status
in recent years. The earliest records of satellite-based AOD are
provided by TOMS (total ozone mapping spectrometer, e.g. Torres et al., 2002)
and AVHRR (Advanced Very High Resolution Radiometer, Geogdzhayev et al.,
2005) from 1979 and 1983 onwards respectively. However, neither one of
these instruments were specifically designed to retrieve aerosol properties.
The more recent dedicated aerosol sounders, such as ATSR (The Along Track
Scanning Radiometer 2, Llewellyn-Jones and Remedios, 2012), MODIS (Moderate
Resolution Imaging Spectroradiometer, Levy et al., 2010), VIISR (Visible
Infrared Imaging Radiometer Suite, Jackson et al., 2013) and MISR
(Multi-angle Imaging SpectroRadiometer, Kahn and Gaitley, 2015) offer data
from 1995, 2000 and 2002 onwards respectively. It is therefore apparent that
neither sun photometer nor satellite records of AOD are available for all the
decades where industrialization has had a significant effect on the aerosol
load.</p>
      <p>There have been, however, recent studies where aerosol load has been
indirectly retrieved from global surface solar radiation (SSR) or separately
from direct and diffuse radiation measurements, which cover much longer time
periods than sun photometer and satellite observations of AOD. Recently, Kudo
et al. (2011) and Lindfors et al. (2013) used radiation measurements taken
with pyranometers and pyrheliometers to estimate AOD. Lindfors et al. (2013)
demonstrated that AOD can be estimated by using SSR and water vapour
information and a look-up table (LUT) generated with a radiative transfer
code. Their method produces AOD estimates that have 2/3 of the results within
<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>20 or <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.05 % of collocated AERONET AODs. Because pyranometer
SSR measurements have been  since 1950s over the globe, the usage of AOD
estimates based on SSR measurements would enable us to construct AOD time
series that go several decades back in time.</p>
      <p>Since the 1990s machine learning methods have made their way to atmospheric
sciences and have been used e.g. in satellite data processing, climate
modelling and weather prediction (Hsieh, 2009). Because of their ability to
retrieve parameters from data that have strongly non-linear relationships,
they have the potential to retrieve AOD from a combination of solar radiation
measurements and auxiliary data such as water vapour content (WVC) and solar
zenith angle (SZA), similarly to what was done by Lindfors et al. (2013)
using a radiative transfer-based approach. The aim of the present work is to
investigate how well machine learning methods are able to estimate AOD from
pyranometer observations by evaluating their performance in comparison with
a radiative transfer-based look-up-table approach. We chose four different
methods: neural network (NN, McCulloch and Pitts, 1943), random forest (RF,
Breiman, 2001), Gaussian process (GP, Santner et al., 2013) and support vector machine (SVM, Smola and Schölkopf, 2004) and compared them against
a look-up table and a non-linear regression method (NR, Bates and Watts,
1988). The performance of these methods was evaluated with AERONET AOD
observations in Thessaloniki, Greece, after the AOD estimates were
derived with SSR observations. Non-linear regression has been successfully
used in multiple studies within aerosol and atmospheric sciences (e.g.
Huttunen et al., 2014; Ahmad et al., 2013). Of these machine learning
methods, neural networks (NNs) have been actively used in different types of
applications in atmospheric sciences. For example, it has been applied to
retrieve aerosol properties from remote sensing instruments (Olcese et al.,
2015; Taylor et al., 2014). Moreover, Foyo-Moreno et al. (2014) uses NNs to
indicate that a ratio between solar diffuse radiation and normal direct
irradiance is the most adequate parameter for estimating AOD from solar
radiation measurements. There have been, however, recent studies where
aerosol load has been indirectly retrieved from global surface solar
radiation (SSR) or separately from direct and diffuse radiation measurements,
which cover much longer time periods than sun photometer and satellite
observations of AOD. Recently, Kudo et al. (2011) and Lindfors et al. (2013)
used radiation measurements taken with pyranometers and pyrheliometers to
estimate AOD. The study by Olcese et al. (2015) is similar to ours in the
sense that they use alternative data together with neural network approach in
an attempt to retrieve AOD at an AERONET site. In their study, they fill in
missing AOD values (e.g. due to cloud cover) at one AERONET station based on
trajectories and AOD observed on another site. To our knowledge, the rest of
the analysed methods have not been used to retrieve aerosol properties
directly from observations.</p>
</sec>
<sec id="Ch1.S2">
  <title>Data and methods</title>
      <p>We compared the ability of several methods to estimate AOD, based on SSR and
water vapour measurements (and SZA that can be readily determined for any
given time and location) against AERONET AOD measurements at 500 nm
(henceforth AOD) taken at Thessalonki, Greece. This site was chosen for this
study, because it has all the necessary high quality measurements from a
10-year time period, because it is the same site to which Lindfors et
al. (2013) applied their LUT approach. Furthermore, the location has varying
aerosol concentrations and relatively high AOD values throughout the year.</p>
<sec id="Ch1.S2.SS1">
  <title>Pyranometer measurements of surface solar radiation</title>
      <p>SSR has been measured at Thessaloniki since January 1993 with a CM21
pyranometer manufactured by Kipp and Zonen. The instrument is located on the
roof of the Physics Department at the Aristotle University of Thessaloniki
(40.63<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 22.96<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E), ca. 60 m above sea level. The data
are sampled every 1–2 s and every minute the average and standard deviation
of the samples are recorded (see more details from Lindfors et al., 2013).
The calibration of the pyranometer has been confirmed to stay within the
quoted manufacturer accuracy (Bais et al., 2013).</p>
</sec>
<sec id="Ch1.S2.SS2">
  <title>AERONET measurements</title>
      <p>AERONET is a network of sun and sky scanning radiometers that measure direct
sun and sky radiance at several wavelengths, typically centred at 340, 380,
440, 500, 670, 870, 940 and 1020 nm, providing measurements of various
aerosol-related properties (Holben et al., 1998). From direct sun
measurements we exploited AOD and WVC data. When sky radiance
measurements are also included, more detailed aerosol properties such as single
scattering albedo (SSA) and asymmetry parameter (gg) can be retrieved
(Dubovik et al., 2000). In the evaluation of the machine learning methods we
used Level 2.0 (cloud-screened and quality assured) AERONET direct sun
measurements of AOD and WVC for Thessaloniki. The Cimel sun photometer is
located on the roof of the Physics Department in the close vicinity of the
pyranometer discussed above. From the inversion products, to interpret some
of our results in more detail, we used level 1.5 (cloud-screened) retrievals.
However, when we selected the data from the Level 1.5 inversion product, we
applied all the other level 2.0 AERONET criteria except for the AOD
threshold. In other words, we applied the same rigorous quality
control that is required for Level 2 data, but we only relaxed the
requirement for AOD at 440 nm to range from 0.4 to 0.1, in order to have
more reliable measurements for our data analysis.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <title>Cloud-screening of the pyranometer measurements and collocation
with the AERONET measurements</title>
      <p>Cloud screening is a crucial factor in the analysis, thus only contribution
of aerosols are considered, not clouds. The SSR data were at first
cloud screened in order to ensure that only clear-sky measurements were
included in the analysis (see Lindfors et al., 2013, for more details).
However, during the analysis of the data it became evident that even after
the initial cloud screening, the SSR data still included observations that
deviated significantly from the main body of the observations. Since there is
a high probability that these outliers in the data were caused e.g.
by cloud contamination, we applied additional screening to the data. Thus, we
removed the clear outliers of possibly undetected clouds, in our case those
observations that deviated by more than <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>20 W m<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> from the
exponential regression fit (SSR <inline-formula><mml:math display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>a</mml:mi><mml:mo>×</mml:mo><mml:mi>exp⁡</mml:mi><mml:mo>(</mml:mo><mml:mo>-</mml:mo><mml:mi>b</mml:mi><mml:mo>×</mml:mo><mml:mtext>AOD</mml:mtext><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:mi>c</mml:mi></mml:mrow></mml:math></inline-formula>, where <inline-formula><mml:math display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math display="inline"><mml:mi>b</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mi>c</mml:mi></mml:math></inline-formula> are regression constants). This additional
screening was applied through regression of SSR against AOD for a given range
of SZA (within <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>). It has to be noted that these data were only
a small fraction of all the data that remained after the cloud screening and
it is very unlikely that the additional cloud screening would affect the main
results and the conclusions of our study.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><caption><p>Statistical characteristics of observed (AERONET) and predicted AOD
by the methods of NR (non-linear regression), LUT (look-up table), NN (neural network), RF (random forest), GP (Gaussian process), SVM (support vector
machine) and some of their combinations (averages without weights, e.g. NN,
SVM combination is their average result). Correlation coefficient (<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:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>,
mean absolute deviation (MAD), median and their <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>20 % percentiles
between the observed and predicted. Time consumptions with a recent
average computer power of the methods for training/estimation in the
magnitude of seconds, minutes and hours. The number of observations is
10 684.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="7">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Method</oasis:entry>  
         <oasis:entry colname="col2">Average(SD)</oasis:entry>  
         <oasis:entry colname="col3"><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></oasis:entry>  
         <oasis:entry colname="col4">MAD</oasis:entry>  
         <oasis:entry colname="col5">Median</oasis:entry>  
         <oasis:entry colname="col6">Fraction in <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>20 %</oasis:entry>  
         <oasis:entry colname="col7">Time consumption</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">AERONET</oasis:entry>  
         <oasis:entry colname="col2">0.240(0.147)</oasis:entry>  
         <oasis:entry colname="col3"/>  
         <oasis:entry colname="col4"/>  
         <oasis:entry colname="col5">0.207</oasis:entry>  
         <oasis:entry colname="col6"/>  
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">NR</oasis:entry>  
         <oasis:entry colname="col2">0.228(0.123)</oasis:entry>  
         <oasis:entry colname="col3">0.880</oasis:entry>  
         <oasis:entry colname="col4">0.053</oasis:entry>  
         <oasis:entry colname="col5">0.210</oasis:entry>  
         <oasis:entry colname="col6">48.4 %</oasis:entry>  
         <oasis:entry colname="col7">seconds/<inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> second</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">LUT</oasis:entry>  
         <oasis:entry colname="col2">0.254(0.136)</oasis:entry>  
         <oasis:entry colname="col3">0.920</oasis:entry>  
         <oasis:entry colname="col4">0.046</oasis:entry>  
         <oasis:entry colname="col5">0.236</oasis:entry>  
         <oasis:entry colname="col6">52.6 %</oasis:entry>  
         <oasis:entry colname="col7">hours/minutes</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">NN</oasis:entry>  
         <oasis:entry colname="col2">0.251(0.156)</oasis:entry>  
         <oasis:entry colname="col3">0.920</oasis:entry>  
         <oasis:entry colname="col4">0.044</oasis:entry>  
         <oasis:entry colname="col5">0.212</oasis:entry>  
         <oasis:entry colname="col6">59.1 %</oasis:entry>  
         <oasis:entry colname="col7">hours/<inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> second</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">RF</oasis:entry>  
         <oasis:entry colname="col2">0.225(0.116)</oasis:entry>  
         <oasis:entry colname="col3">0.870</oasis:entry>  
         <oasis:entry colname="col4">0.052</oasis:entry>  
         <oasis:entry colname="col5">0.204</oasis:entry>  
         <oasis:entry colname="col6">52.9 %</oasis:entry>  
         <oasis:entry colname="col7">tens of seconds/<inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> second</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">GP</oasis:entry>  
         <oasis:entry colname="col2">0.240(0.130)</oasis:entry>  
         <oasis:entry colname="col3">0.927</oasis:entry>  
         <oasis:entry colname="col4">0.041</oasis:entry>  
         <oasis:entry colname="col5">0.213</oasis:entry>  
         <oasis:entry colname="col6">60.8 %</oasis:entry>  
         <oasis:entry colname="col7">minutes/tens of seconds</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SVM</oasis:entry>  
         <oasis:entry colname="col2">0.242(0.150)</oasis:entry>  
         <oasis:entry colname="col3">0.918</oasis:entry>  
         <oasis:entry colname="col4">0.044</oasis:entry>  
         <oasis:entry colname="col5">0.201</oasis:entry>  
         <oasis:entry colname="col6">58.4 %</oasis:entry>  
         <oasis:entry colname="col7">tens of seconds/<inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> second</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">NN, SVM</oasis:entry>  
         <oasis:entry colname="col2">0.247(0.152)</oasis:entry>  
         <oasis:entry colname="col3">0.924</oasis:entry>  
         <oasis:entry colname="col4">0.043</oasis:entry>  
         <oasis:entry colname="col5">0.207</oasis:entry>  
         <oasis:entry colname="col6">59.7 %</oasis:entry>  
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">NN, SVM, RF</oasis:entry>  
         <oasis:entry colname="col2">0.240(0.138)</oasis:entry>  
         <oasis:entry colname="col3">0.922</oasis:entry>  
         <oasis:entry colname="col4">0.042</oasis:entry>  
         <oasis:entry colname="col5">0.205</oasis:entry>  
         <oasis:entry colname="col6">59.9 %</oasis:entry>  
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SVM, RF</oasis:entry>  
         <oasis:entry colname="col2">0.234(0.131)</oasis:entry>  
         <oasis:entry colname="col3">0.913</oasis:entry>  
         <oasis:entry colname="col4">0.044</oasis:entry>  
         <oasis:entry colname="col5">0.202</oasis:entry>  
         <oasis:entry colname="col6">58.0 %</oasis:entry>  
         <oasis:entry colname="col7"/>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">NN, RF</oasis:entry>  
         <oasis:entry colname="col2">0.238(0.134)</oasis:entry>  
         <oasis:entry colname="col3">0.916</oasis:entry>  
         <oasis:entry colname="col4">0.043</oasis:entry>  
         <oasis:entry colname="col5">0.207</oasis:entry>  
         <oasis:entry colname="col6">59.0 %</oasis:entry>  
         <oasis:entry colname="col7"/>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p>The SSR values were collocated for each AOD with the <inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>1 min difference,
averaged and finally normalized for the Sun–Earth distance corresponding to
1 January. The training data set for the machine learning methods contained
the years 2009–2014 and the validation (verification) data set years 2005–2008.
These periods were selected because we wanted to verify whether the methods could
provide reasonable AOD estimates for a period other than the training period.
The training data set covered approximately 2/3 and the validation data set
1/3 of the whole data. For all methods the input parameters are SSR, WVC
and SZA and they produce AOD estimates. Table A1 in Appendix A summarizes
the statistics of maximum, minimum, average, SD and median for the input and
the output parameters. Table A1 shows that AOD is larger for the
validation data set, although the maximum value is larger for the training.</p>
</sec>
<sec id="Ch1.S2.SS4">
  <title>LUT and NR methods for AOD retrievals</title>
<sec id="Ch1.S2.SS4.SSS1">
  <title>Radiative transfer model based look-up table (LUT)</title>
      <p>To retrieve AOD from SSR observations Lindfors et al. (2013) produced a LUT
based on radiative transfer simulations. They simulated SSR in different
atmospheric conditions by varying AOD, WVC and SZA systematically. They used
a single aerosol model for all the simulations, and therefore called their
AOD estimate as an effective AOD, which is only a function of SSR, SZA and WVC.
Other parameters were assumed as constants, e.g. Ångström Exponent of
1.1, SSA at 500 nm of 0.92 (the SSA's spectral pattern follows the rural
background aerosol model by Shettle (1989), where SSA changes from roughly
0.92 at 400 nm to 0.89 at 1000 nm). The asymmetry parameter was assumed
wavelength independent with a value of 0.68, while the albedo was varying with
wavelength and SZA. For a more detailed description of the LUT method see
Lindfors et al. (2013).</p>
</sec>
<sec id="Ch1.S2.SS4.SSS2">
  <title>Non-linear regression method (NR)</title>
      <p>The non-linear regression (NR) is a multivariate analysis method which is
used when the dependencies between the study variables are not linear (Bates
and Watts, 1988). NR is useful especially when there are physical reasons
for believing that the relationship between the response and the predictors
follows a particular functional form. Benefits of NR are that it needs only
moderate-sized samples of the studied phenomena to give adequately precise
results and as an output it gives a simple but not predefined function for
prediction. An additional advantage of NR against the other methods presented
in this paper is that once the parameters are estimated, they can be used in
similar cases without additional training data. In this study we assume that
AOD can be estimated as a function of SSR, WVC and SZA. Multiple different
formulations for the NR function were tested and the function with the best
prediction ability found for this data is given by

                  <disp-formula specific-use="align" content-type="numbered"><mml:math display="block"><mml:mtable displaystyle="true"><mml:mtr><mml:mtd><mml:mrow><mml:mtext>AOD</mml:mtext></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mtext>exp</mml:mtext><mml:mfenced open="(" close=")"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mtext>SZA</mml:mtext></mml:mfrac></mml:mstyle></mml:mfenced><mml:mo>+</mml:mo><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mtext>exp</mml:mtext><mml:mfenced open="(" close=")"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mtext>SSR</mml:mtext></mml:mfrac></mml:mstyle></mml:mfenced></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>+</mml:mo><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mtext>exp</mml:mtext><mml:mfenced open="(" close=")"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mtext>WVC</mml:mtext></mml:mfrac></mml:mstyle></mml:mfenced><mml:mo>+</mml:mo><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mtext>exp</mml:mtext><mml:mfenced close=")" open="("><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mtext>SZA</mml:mtext></mml:mfrac></mml:mstyle><mml:mo>+</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mtext>SSR</mml:mtext></mml:mfrac></mml:mstyle></mml:mfenced></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>+</mml:mo><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">5</mml:mn></mml:msub><mml:mi>exp⁡</mml:mi><mml:mfenced open="(" close=")"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mtext>SZA</mml:mtext></mml:mfrac></mml:mstyle><mml:mo>+</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mtext>WVC</mml:mtext></mml:mfrac></mml:mstyle></mml:mfenced></mml:mrow></mml:mtd></mml:mtr><mml:mlabeledtr id="Ch1.E1"><mml:mtd/><mml:mtd/><mml:mtd><mml:mrow><mml:mo>+</mml:mo><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">6</mml:mn></mml:msub><mml:mi>exp⁡</mml:mi><mml:mfenced open="(" close=")"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mtext>SSR</mml:mtext></mml:mfrac></mml:mstyle><mml:mo>+</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mtext>WVC</mml:mtext></mml:mfrac></mml:mstyle></mml:mfenced><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

              The coefficients <inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>–<inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">6</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> were determined using R-software (R Core Team,
2014) and are shown in Table A2.</p>
</sec>
</sec>
<sec id="Ch1.S2.SS5">
  <title>Machine learning methods for AOD retrievals</title>
<sec id="Ch1.S2.SS5.SSS1">
  <title>Neural network (NN)</title>
      <p>Artificial neural networks belong to the family of machine learning methods
(McCulloch and Pitts, 1943). As usual in machine learning methods, the aim of
an artificial NN is to generate a mathematical model to represent the
phenomenon that is examined. The mathematical model of NN structure
specifically consists of interconnected neurons with numeric weights. A
typical NN model is multilayer perceptron (MLP) (Rosenblatt, 1958), which is
used in this study. A MLP network consists of several neuron layers: an input
layer, hidden layers and an output layer. The weights and other parameters of
the model are tuned or trained with a specific training data set containing
input–output pairs of the phenomenon. In this case the model inputs are SSR,
WVC and SZA, and the output is AOD. The training is executed with a training
algorithm and in this paper the Levenberg–Marquardt algorithm is used (Hagan
and Menhaj, 1994). A total of 20 NNs were trained in this case. The NNs
differed from each other by the number of neurons in a hidden layer. Five
networks with the smallest prediction error within the training data set were
selected to the final committee of networks. The final prediction of the NN
model was computed as a median of the outputs of all networks in the
committee. For more information on NNs see, for example, Bishop (1995).</p>
</sec>
<sec id="Ch1.S2.SS5.SSS2">
  <title>Random forest (RF)</title>
      <p>Random forest is a machine learning technique that may be used for
classification and non-linear regression (Breiman, 2001). RF for non-linear
regression consists of an ensemble of binary regression trees. Each of these
trees is constructed using a randomized training scheme and is essentially a
piecewise constant fit to the training data set. The prediction of a RF model
is obtained by averaging the regression tree predictions over the whole model
ensemble. In this study, the RF implementation from the Scikit–Learn machine
learning library (Pedregosa et al., 2011) was used. We used (SSR, WVC, SZA,
SSRxWVC, SSWxSZA, WVCxSZA) as the RF model inputs and AOD as the output. A
randomized cross-validation scheme was used to find the optimal training
parameters for the RF. For more information on RFs see, for example, Friedman
et al. (2001).</p>
</sec>
<sec id="Ch1.S2.SS5.SSS3">
  <title>Support vector machine (SVM)</title>
      <p>Support vector machine (SVM) is a machine learning technique (Vapnik, 1995;
Burges, 1998). In this study, we use the standard SVM regression (SVR), the
formulation based on the commonly used <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">ε</mml:mi></mml:math></inline-formula>-SVR with radial basis
kernel function. For implementing the SVM the libsvm package was used (Chang
and Lin, 2011). The objective of <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">ε</mml:mi></mml:math></inline-formula>-SVR is to find a function
that has at most <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">ε</mml:mi></mml:math></inline-formula> deviation from the training data set outputs.
The training of an <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">ε</mml:mi></mml:math></inline-formula>-SVR model is formulated as a quadratic
(convex) optimization problem in which the Vapnik's <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">ε</mml:mi></mml:math></inline-formula>-insensitive loss function is minimized (e.g. Vapnik, 1995). The
<inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">ε</mml:mi></mml:math></inline-formula>-SVR model has two training parameters that were used to
control the training: the regularization parameter, which controls the
smoothness of the approximation function (sensitivity to noise) and the
parameter <inline-formula><mml:math display="inline"><mml:mi mathvariant="italic">ε</mml:mi></mml:math></inline-formula>, which dominates the number of support vectors by
governing the accuracy of the approximation function. The determination of
SVM control parameters was solved by the means of a grid search. For a more
detailed description of the method, the reader is referred to
Smola and Schölkopf (2004).</p>
</sec>
<sec id="Ch1.S2.SS5.SSS4">
  <title>Gaussian process (GP)</title>
      <p>Gaussian process (GP) for machine learning is a generic supervised learning
method that may be used, for example, for non-linear regression. In GP
learning, the function inputs and outputs are treated as Gaussian random
variables and the correlations between these variables are modelled. The
predictions given by a GP model are computed as conditional probability
distributions given the training data and function inputs. As the prediction
given by a GP model is a probability distribution, the error estimates for
the predicted point estimates are obtained automatically. In this study, the
GP implementation from the Scikit–Learn machine learning library was used.
The same inputs and output variables as with the RF models were used in the
GP training. The best performing correlation function training parameters
were sought for using maximum likelihood estimation. A total of 25 GP models
were trained. The training of each model was carried out using 2500 training
data samples that were randomly sampled from the full training data set. The
five best performing GP models were selected into the final GP model
committee. The final prediction was computed as the median of the predictions
given by the GP models in the committee. For more information on GPs for
machine learning see, for example, Welch et al. (1992), Rasmussen and
Williams (2006), and Santner et al. (2013).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><caption><p>Observed (AERONET) and predicted AOD using the methods of <bold>(a)</bold> LUT
(look-up table), <bold>(b)</bold> GP (Gaussian process), <bold>(c)</bold> NN (neural network) and <bold>(d)</bold> SVM
(support vector machine). The colourbar indicates the absolute number of
results in the areas with the interval of 0.01 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.01. The 1 : 1 lines and
linear fits included. The number of observations is 10 684. The relation for
the linear fits is estimated AOD <inline-formula><mml:math display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>a</mml:mi><mml:mn mathvariant="normal">1</mml:mn><mml:mo>+</mml:mo><mml:mi>a</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> AERONET AOD, and the
coefficients of the least square fits with their errors are (<inline-formula><mml:math display="inline"><mml:mrow><mml:mi>a</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math display="inline"><mml:mrow><mml:mi>a</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>):
0.050(<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.001), 0.849(<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.004); 0.043(<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.001),
0.820(<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.003); 0.016(<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.001), 0.979(<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.004) and
0.018(<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.001), 0.936(<inline-formula><mml:math display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula>0.004), for LUT, GP, NN and SVM respectively.</p></caption>
            <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016-f01.png"/>

          </fig>

</sec>
</sec>
</sec>
<sec id="Ch1.S3">
  <title>Results</title>
<sec id="Ch1.S3.SS1">
  <title>Comparison of the methods</title>
      <p>Table 1 shows the statistics of the AOD observed by AERONET together with the
statistical characteristics of the predicted AOD for the years 2005–2008.
From the table, we can see that predicted values show good correlation
against the observations for all the methods. Predictions by RF had the
lowest correlation coefficient with a value of 0.87 while the correlation
coefficient for NR was only slightly larger, 0.88. For the best performing
methods, LUT, GP, NN and SVM, the correlation coefficients were
approximately 0.92. Their predicted AODs in comparison to AERONET AOD are
shown in Fig. 1. To visualize the distribution of the data, the colourbar in
Fig. 1 represents the number of observations for each AOD interval of 0.005.
Based on the different statistics in Table 1, machine learning methods (NN,
SVM, GP) produce a good match with AERONET data and they perform equally well
or better than the LUT method according to all the metrics. Due to the fact
that RF and NR are not able to produce as good estimates as the LUT method,
they were left out from the more detailed analysis.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><caption><p>Differences between predicted and observed (AERONET) AOD for the
methods: <bold>(a)</bold> LUT (look-up table), <bold>(b)</bold> GP (Gaussian process), <bold>(c)</bold> NN (neural network) and <bold>(d)</bold> SVM (support vector machine) with respect to the observed
AOD. The crosses indicate the means of each subgroup, the limits of the
boxes are 25, 50 and 75 % of the data, and the lines are
plotted with 1.5 times the interquartile ranges.</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016-f02.pdf"/>

        </fig>

      <p>Although these methods are able to predict the average AOD with a good
accuracy, they differ when we compare their ability to predict different AOD
levels. In Fig. 1, the colourbar indicates the absolute number of results
in the areas with the interval of 0.01 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.01 (vertically and
horizontally) for AOD; in addition 1 : 1 lines and linear fits are
included. Based on the linear fits, NN appears to have the best agreement
with AERONET data for the whole AOD range. As the average and median values
of AERONET AOD are 0.240 and 0.207 respectively (Table 1), the main
population of the measurements is in the range of moderate AODs. The machine
learning methods are obviously weighted to perform best in this range of
AODs. However, from Fig. 2, which shows the absolute difference between
AERONET and predicted AOD, we can see that LUT and GP tend to significantly
underestimate AOD for AODs larger than 0.5, while NN and SVM are able to
reach smaller differences with AERONET on average, although with larger
overall variabilities than LUT and GP. Although NN and SVM also start to
deviate from the observations at higher AODs, these deviations are more
modest in a relative sense as can be seen from Fig. 3, which shows the relative
difference between the observations and predictions. All the methods
overestimate AOD in relative terms when AOD approaches zero (Fig. 3).
However, as Fig. 2 demonstrates, the absolute error is systematically very
low in the small AOD region (AOD <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 0.2). NN and SVM are generalized
better for large AODs than the other methods, where the amount of data are
small.</p>
      <p><?xmltex \hack{\newpage}?>In Table 1, the four last rows represent the values for cases where
the results of machine learning methods are combined by averaging them. As
can be seen from the table, these combinations do not improve the estimates
compared to the statistical values of individual methods.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><caption><p>The same as Fig. 2, but the vertical axis indicates the ratio of the
predicted to the observed (AERONET) AOD.</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016-f03.pdf"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS2">
  <title>The effect of water vapour on AOD predictions</title>
      <p>Huttunen et al. (2014) showed that WVC and AOD typically have a positive
correlation. Therefore, we investigated how the AOD estimates from different
methods are affected by WVC. Figure 4 shows the relative difference between
the predictions and measured AOD with respect to WVC. From this figure, we
can see that the LUT-based AODs are overestimated at the smallest and
underestimated at the largest WVC contents. The reason for this behaviour is
that the LUT method has been set to assume prescribed and constant properties
for many relevant parameters that affect SSR (other than AOD and WVC); e.g.
aerosol single scattering albedo, asymmetry parameter and surface albedo
(Lindfors et al., 2013). Consequently, the assumption of constant SSA in
particular leads to WVC-dependent systematic bias of the LUT-based AOD, as we
will show next. The other methods are closer to the ratio of 1 without such a
systematic bias, excluding the SVM underestimation for the smallest WVC.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><caption><p>The same as Fig. 3, but the ratio of predicted to measured AOD is
given as a function of the water vapour content (WVC).</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016-f04.pdf"/>

        </fig>

      <p>Figure 5 shows measured SSR and LUT-based SSR for a narrow set of SZAs
(48.50–51.50<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>). AOD is on the horizontal axis, SSR on the vertical
axis and WVC is shown with the colourbar. From Fig. 5a it is evident that LUT
incorporates a strong WVC-dependent structure: for a given SSR level, AOD
decreases with increasing water vapour content. This pattern follows from the
assumption that the aerosol composition remains the same, i.e. it has a fixed
SSA value. Thus in the LUT method, increases in SSR absorption by water
vapour are compensated by decreases in aerosol extinction. In the real
atmosphere, water vapour content also has implications on aerosol composition
and size. If all conditions apart from water vapour remained constant,
increase of water vapour would also increase the uptake of water into aerosol
particles thus affecting the aerosol SSA. The effect of fixed SSA is also
visible in the way the LUT-based AOD estimates are distributed (Fig. 5a). In
Figure 5c we can see that for a given AOD in the LUT, the highest WVC values
always correspond to the lowest SSR values. However, the same pattern is not
clearly visible either in the plot with the measured values (Fig. 5b) or in
the plot with AOD from NN (Fig. 5d). This indicates that although the machine
learning methods do not explicitly get any information about the possible
systematic covariability of WVC and SSA, they seem to be able to detect it
indirectly, at least to some extent.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><caption><p>Solar surface radiation (SSR), aerosol optical depth (AOD) and
water vapour content (WVC) for a fixed solar zenith angle (48.50–51.50<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>) for <bold>(a)</bold> look-up table (LUT) and <bold>(b)</bold> measurements (Meas).
The predicted AODs for <bold>(c)</bold> LUT and <bold>(d)</bold> neural network (NN) are the
same for SSR, WVC and SZA.</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016-f05.pdf"/>

        </fig>

      <p>To further illustrate this, Fig. 6a shows the AERONET measurements of AOD and
single scattering co-albedo, 1-SSA at 500 nm as a function of WVC. Here,
together with the absorption strength by the water vapour, we considered more
illustrative to show the single scattering co-albedo rather than SSA. In this
plot, SZA, SSR and season were limited respectively to
58<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> SZA <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 62<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>,
420 W m<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> SSR <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 460 W m<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, June–August, allowing
enough data with the limited parameters. Thus, the plot illustrates the
co-variability of WVC and SSA for a limited range of surface solar radiation
and SZA, for conditions when the LUT method produces lower AOD values for
higher WVC (Fig. 5a). However, Fig. 6a clearly shows that an opposite
relationship between AOD and WVC is obtained by the measurements. Moreover,
this pattern is compensated by aerosol absorption (remember that in this
subset we constrained SSR), which decreases with increasing WVC; this is
likely related to the aerosol swelling by hygroscopic growth that increases
the scattering of the aerosol. Therefore, we can conclude from the
measurements that because of the covariability of WVC and SSA in
Thessaloniki, the assumption of a fixed SSA in the LUT causes limitations for
predicting AOD, while the machine learning methods can take into account, at
least to some extent, this relationship indirectly. Using radiative transfer
modelling we demonstrated the magnitude of these changes in water vapour
and aerosol absorption, as indicated in Fig. 6. Indeed, they induced opposite
effects of similar magnitude in surface solar irradiance. For the base case,
we simulated SSR with WVC of 2.8 cm and 1-SSA of 0.06 (with SZA of
60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> and AOD of 0.3) as inputs, resulting in 439.9 W m<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. When
we increased the water vapour column to 3.6 cm, the corresponding decrease
in SSR was about 6.8 W m<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. However, when we additionally decreased
the aerosol absorption (1-SSA) to 0.04, the difference to the base case
shrank to 1.8 W m<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and this remaining amount can mostly be explained
by the asymmetry parameter, which also exhibits a systematic dependence with
WVC (stronger forward scattering by particles grown in humid conditions).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6"><caption><p><bold>(a)</bold> Aerosol optical depth (AOD), water vapour content (WVC) and 1-SSA
at 500 nm from the AERONET inversion sky data. <bold>(b)</bold> SSA at 500 nm, WVC and the
LUT's predicted AOD divided with the observational AOD (AERONET), with the
red line fixed to SSA (500 nm) <inline-formula><mml:math display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 0.92 (as in LUT).</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/16/8181/2016/acp-16-8181-2016-f06.pdf"/>

        </fig>

      <p>The lower panel of Fig. 6 further illustrates the role of fixed SSA in the
observed WVC-dependent bias in the LUT results, which can be avoided with the
machine learning methods. It shows the mean ratio of LUT-estimated and
AERONET-measured AOD on the right-hand side <inline-formula><mml:math display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axis as a function of water
vapour content (so essentially the same results shown by a box-plot in
Fig. 4). Additionally, on the left-hand side <inline-formula><mml:math display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axis, the single scattering
albedo (estimated for 500 nm) from AERONET measurements is shown as a
function of water vapour amount as well. This also demonstrates that the
over- and underestimations of the LUT method coincide with SSA range that is
under and over the assumed fixed value of 0.92 (shown with red dashed line) respectively. Visibly, the ratio in the right-hand axis of Fig. 6b, reaches
one not until SSA is roughly 0.93 instead of 0.92. Presumably, SSA has
actually a different wavelength pattern than the one assumed in LUT.</p>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <title>Conclusions</title>
      <p>We have used several inverse methods to retrieve aerosol optical depth (AOD)
from surface solar radiation (SSR) and water vapour content (WVC)
measurements (with corresponding solar zenith angle data) taken in
Thessaloniki, Greece. Two traditional (look-up table and non-linear
regression) and four machine learning methods (Gaussian process,
neural network, random forest and support vector machine)
were used to retrieve AOD estimates for the years 2005–2008. Then we
compared the AOD estimates with collocated AOD measurements by Aerosol
Robotic Network (AERONET). Our comparisons showed the following.</p>
      <p><?xmltex \hack{\newpage}?>AOD estimates based on the LUT method agreed better with AERONET than the NR
estimates but apart from RF, the machine learning methods produced AOD
estimates that were comparable or better than LUT.</p>
      <p>NN and SVM methods reproduced good correspondence to AERONET observations
for both low and high AODs while the rest of the methods tended to overestimate
low AODs and underestimate high AODs. The main reason for the better
performance of these machine learning methods was that there were no
constraints of the aerosol single scattering albedo (SSA) in the retrieval.
In other words, the methods do not need to explicitly make assumptions on
the optical aerosol properties of the atmosphere because they seem to be able
to indirectly account for the covariation of WVC and SSA.</p>
      <p>When compared with AERONET measurements, the best AOD estimates were
retrieved with the machine learning algorithms, but only NN and SVM were also
able to generalize accurate estimates for large AODs.</p>
      <p>The machine learning methods are sensitive to the selection of the training
data set and other constraints, and are generally valid only for the range
of variables used for their training; thus care needs to be taken when
these methods are employed.</p>
      <p>These tools have the potential to be used in the retrieval of AOD from SSR
measurements to lengthen the time series of AOD. Historical AOD is essential
in the estimation of anthropogenic aerosol effects and in the evaluation of
AOD retrievals from space-borne instruments before the 1990s.</p>
      <p>The intention of comparing different methods was to test their ability in an
“out-of-the-box” configuration. With this in mind, methods were not
particularly tuned to reach the best possible results. It is very likely that
e.g. optimizing the free parameters used in each of the non-linear modelling
approaches, their ability to reproduce observed AOD could be further
improved.</p><?xmltex \hack{\clearpage}?>
</sec>

      
      </body>
    <back><app-group>

<app id="App1.Ch1.S1">
  <title/>

<?xmltex \floatpos{h!}?><table-wrap id="App1.Ch1.T1"><?xmltex \hack{\hsize\textwidth}?><caption><p>The statistics between the training and the validation data for
the input and the output parameters. The units for SZA, SSR and WVC are
degrees, W m<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and centimetres respectively.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="6">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:thead>
       <oasis:row>  
         <oasis:entry colname="col1">Training:</oasis:entry>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3"/>  
         <oasis:entry colname="col4"/>  
         <oasis:entry colname="col5"/>  
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Parameter</oasis:entry>  
         <oasis:entry colname="col2">Max</oasis:entry>  
         <oasis:entry colname="col3">Min</oasis:entry>  
         <oasis:entry colname="col4">Average</oasis:entry>  
         <oasis:entry colname="col5">SD</oasis:entry>  
         <oasis:entry colname="col6">Median</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">SZA</oasis:entry>  
         <oasis:entry colname="col2">78.6</oasis:entry>  
         <oasis:entry colname="col3">17.5</oasis:entry>  
         <oasis:entry colname="col4">56.2</oasis:entry>  
         <oasis:entry colname="col5">15.7</oasis:entry>  
         <oasis:entry colname="col6">60.0</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SSR</oasis:entry>  
         <oasis:entry colname="col2">1071.9</oasis:entry>  
         <oasis:entry colname="col3">120.5</oasis:entry>  
         <oasis:entry colname="col4">522.7</oasis:entry>  
         <oasis:entry colname="col5">247.1</oasis:entry>  
         <oasis:entry colname="col6">479.6</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">WVC</oasis:entry>  
         <oasis:entry colname="col2">4.12</oasis:entry>  
         <oasis:entry colname="col3">0.23</oasis:entry>  
         <oasis:entry colname="col4">2.23</oasis:entry>  
         <oasis:entry colname="col5">0.73</oasis:entry>  
         <oasis:entry colname="col6">2.29</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">AOD</oasis:entry>  
         <oasis:entry colname="col2">1.06</oasis:entry>  
         <oasis:entry colname="col3">0.01</oasis:entry>  
         <oasis:entry colname="col4">0.22</oasis:entry>  
         <oasis:entry colname="col5">0.12</oasis:entry>  
         <oasis:entry colname="col6">0.20</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">Validation:</oasis:entry>  
         <oasis:entry colname="col2"/>  
         <oasis:entry colname="col3"/>  
         <oasis:entry colname="col4"/>  
         <oasis:entry colname="col5"/>  
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Parameter</oasis:entry>  
         <oasis:entry colname="col2">Max</oasis:entry>  
         <oasis:entry colname="col3">Min</oasis:entry>  
         <oasis:entry colname="col4">Average</oasis:entry>  
         <oasis:entry colname="col5">SD</oasis:entry>  
         <oasis:entry colname="col6">Median</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SZA</oasis:entry>  
         <oasis:entry colname="col2">78.7</oasis:entry>  
         <oasis:entry colname="col3">17.5</oasis:entry>  
         <oasis:entry colname="col4">60.6</oasis:entry>  
         <oasis:entry colname="col5">14.7</oasis:entry>  
         <oasis:entry colname="col6">65.3</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">SSR</oasis:entry>  
         <oasis:entry colname="col2">1060.0</oasis:entry>  
         <oasis:entry colname="col3">113.2</oasis:entry>  
         <oasis:entry colname="col4">450.2</oasis:entry>  
         <oasis:entry colname="col5">235.9</oasis:entry>  
         <oasis:entry colname="col6">384.5</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">WVC</oasis:entry>  
         <oasis:entry colname="col2">3.81</oasis:entry>  
         <oasis:entry colname="col3">0.27</oasis:entry>  
         <oasis:entry colname="col4">1.87</oasis:entry>  
         <oasis:entry colname="col5">0.82</oasis:entry>  
         <oasis:entry colname="col6">1.79</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">AOD</oasis:entry>  
         <oasis:entry colname="col2">0.85</oasis:entry>  
         <oasis:entry colname="col3">0.03</oasis:entry>  
         <oasis:entry colname="col4">0.24</oasis:entry>  
         <oasis:entry colname="col5">0.15</oasis:entry>  
         <oasis:entry colname="col6">0.21</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

<?xmltex \floatpos{h!}?><table-wrap id="App1.Ch1.T2"><?xmltex \hack{\hsize\textwidth}?><caption><p>The coefficient values of Eq. (1) and errors (SD) for the NR
method.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="3">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">Coefficients</oasis:entry>  
         <oasis:entry colname="col2">Estimate</oasis:entry>  
         <oasis:entry colname="col3">SD error</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1"><inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2">1.716 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">5</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3">8.372 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"><inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.696 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">5</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3">8.272 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"><inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.715 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">5</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3">8.363 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"><inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2"><inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>1.206 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3">5.727 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"><inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2">1.694 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">5</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3">8.264 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"><inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">5</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2">5.145 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">0</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3">2.465 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1"><inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mn mathvariant="normal">6</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col2">6.819 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">0</mml:mn></mml:msup></mml:math></inline-formula></oasis:entry>  
         <oasis:entry colname="col3">3.728 <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

<?xmltex \hack{\clearpage}?>
</app>
  </app-group><ack><title>Acknowledgements</title><p>We thank the AERONET team, principal investigators and other participants for
their effort in establishing and maintaining the network. This study is
supported by Graduate school in Physics, Chemistry, Biology and Meteorology
of Atmospheric Composition and Climate Change: From Molecular Processes to
Global Observations and Models. The Academy of Finland Center of Excellence
program (project number 272041) is also acknowledged. The financial support
by the strategic funding of the University of Eastern Finland is gratefully
acknowledged. The author thank Juha Tonttila and Mikko Pitkänen from
Finnish Meteorological Institute, Kuopio, for their help with the python
(<uri>http://python.org</uri>) and in the production of the MatLab
(<uri>http://mathworks.com</uri>) box plot figures. Also J. Huttunen thank the
Finnish Cultural Foundation, North Savo Regional fund.<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?> Edited by: B. Mayer</p></ack><ref-list>
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    <!--<article-title-html>Retrieval of aerosol optical depth from surface solar radiation measurements
using machine learning algorithms, non-linear regression and a radiative
transfer-based look-up table</article-title-html>
<abstract-html><p class="p">In order to have a good estimate of the current forcing by anthropogenic
aerosols, knowledge on past aerosol levels is needed. Aerosol optical depth
(AOD) is a good measure for aerosol loading. However, dedicated measurements
of AOD are only available from the 1990s onward. One option to lengthen the AOD
time series beyond the 1990s is to retrieve AOD from surface solar radiation
(SSR) measurements taken with pyranometers. In this work, we have evaluated
several inversion methods designed for this task. We compared a look-up
table method based on radiative transfer modelling, a non-linear regression
method and four machine learning methods (Gaussian process, neural network,
random forest and support vector machine) with AOD observations carried out with a
sun photometer at an Aerosol Robotic Network (AERONET) site in Thessaloniki,
Greece. Our results show that most of the machine learning methods produce
AOD estimates comparable to the look-up table and non-linear regression
methods. All of the applied methods produced AOD values that corresponded
well to the AERONET observations with the lowest correlation coefficient
value being 0.87 for the random forest method. While many of the methods
tended to slightly overestimate low AODs and underestimate high AODs, neural network and support vector machine showed overall better correspondence for
the whole AOD range. The differences in producing both ends of the AOD range
seem to be caused by differences in the aerosol composition. High AODs were
in most cases those with high water vapour content which might affect the
aerosol single scattering albedo (SSA) through uptake of water into
aerosols. Our study indicates that machine learning methods benefit from the
fact that they do not constrain the aerosol SSA in the retrieval, whereas
the LUT method assumes a constant value for it. This would also mean that
machine learning methods could have potential in reproducing AOD from SSR
even though SSA would have changed during the observation period.</p></abstract-html>
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