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  <front>
    <journal-meta><journal-id journal-id-type="publisher">ACP</journal-id><journal-title-group>
    <journal-title>Atmospheric Chemistry and Physics</journal-title>
    <abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys.</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">1680-7324</issn><publisher>
    <publisher-name>Copernicus Publications</publisher-name>
    <publisher-loc>Göttingen, Germany</publisher-loc>
  </publisher></journal-meta>
    <article-meta>
      <article-id pub-id-type="doi">10.5194/acp-18-11247-2018</article-id><title-group><article-title>Intra-annual variations of regional aerosol optical depth, vertical
distribution, and particle types from multiple satellite and ground-based
observational datasets</article-title><alt-title>Intra-annual variations of aerosol loading and
properties</alt-title>
      </title-group><?xmltex \runningtitle{Intra-annual variations of aerosol loading and
properties}?><?xmltex \runningauthor{B. Zhao et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Zhao</surname><given-names>Bin</given-names></name>
          <email>zhaob1206@ucla.edu</email>
        <ext-link>https://orcid.org/0000-0001-8438-9188</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Jiang</surname><given-names>Jonathan H.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-5929-8951</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Diner</surname><given-names>David J.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Su</surname><given-names>Hui</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Gu</surname><given-names>Yu</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-3412-0794</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Liou</surname><given-names>Kuo-Nan</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Jiang</surname><given-names>Zhe</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Huang</surname><given-names>Lei</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Takano</surname><given-names>Yoshi</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Fan</surname><given-names>Xuehua</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Omar</surname><given-names>Ali H.</given-names></name>
          
        </contrib>
        <aff id="aff1"><label>1</label><institution>Joint Institute for Regional Earth System Science and Engineering and
Department of Atmospheric and Oceanic Sciences, University of California,
Los Angeles, California, USA</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Jet propulsion Laboratory, California Institute of Technology,
Pasadena, California, USA</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>NASA Langley Research Center, Hampton, Virginia, USA</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Bin Zhao (zhaob1206@ucla.edu)</corresp></author-notes><pub-date><day>13</day><month>August</month><year>2018</year></pub-date>
      
      <volume>18</volume>
      <issue>15</issue>
      <fpage>11247</fpage><lpage>11260</lpage>
      <history>
        <date date-type="received"><day>31</day><month>January</month><year>2018</year></date>
           <date date-type="rev-request"><day>12</day><month>April</month><year>2018</year></date>
           <date date-type="rev-recd"><day>12</day><month>June</month><year>2018</year></date>
           <date date-type="accepted"><day>27</day><month>July</month><year>2018</year></date>
      </history>
      <permissions>
        
        
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://acp.copernicus.org/articles/.html">This article is available from https://acp.copernicus.org/articles/.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/.pdf</self-uri>
      <abstract>
    <p id="d1e185">The climatic and health effects of aerosols are strongly dependent on the
intra-annual variations in their loading and properties. While the seasonal
variations of regional aerosol optical depth (AOD) have been extensively
studied, understanding the temporal variations in aerosol vertical
distribution and particle types is also important for an accurate estimate of
aerosol climatic effects. In this paper, we combine the observations from
four satellite-borne sensors and several ground-based networks to investigate
the seasonal variations of aerosol column loading, vertical distribution, and
particle types over three populous regions: the Eastern United States (EUS),
Western Europe (WEU), and Eastern and Central China (ECC). In all three
regions, column AOD, as well as AOD at heights above 800 m, peaks in
summer/spring, probably due to accelerated formation of secondary aerosols
and hygroscopic growth. In contrast, AOD below 800 m peaks in winter over
WEU and ECC regions because more aerosols are confined to lower heights due
to the weaker vertical mixing. In the EUS region, AOD below 800 m shows two
maximums, one in summer and the other in winter. The temporal trends in
low-level AOD are consistent with those in surface fine particle
(PM<inline-formula><mml:math id="M1" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula>) concentrations. AOD due
to fine particles (<inline-formula><mml:math id="M2" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.7</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M3" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter) is much larger in
spring/summer than in winter over all three regions. However, the coarse mode
AOD (<inline-formula><mml:math id="M4" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">1.4</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M5" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter), generally shows small variability,
except that a peak occurs in spring in the ECC region due to the prevalence
of airborne dust during this season. When aerosols are classified according
to sources, the dominant type is associated with anthropogenic air pollution,
which has a similar seasonal pattern as total AOD. Dust and sea-spray
aerosols in the WEU region peak in summer and winter, respectively, but do
not show an obvious seasonal pattern in the EUS region. Smoke aerosols, as
well as absorbing aerosols, present an obvious unimodal distribution with a
maximum occurring in summer over the EUS and WEU regions, whereas they follow
a bimodal distribution with peaks in August and March (due to crop residue
burning) over the ECC region.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p id="d1e238">Aerosols have adverse effects on human health  (Lelieveld et al.,
2015) and play a key role in Earth's climate through aerosol–radiation
interactions (McCormick and Ludwig, 1967) and aerosol–cloud
interactions (Twomey, 1977; Albrecht, 1989; Garrett and Zhao, 2006).
Compared with long-lived climate forcers such as <inline-formula><mml:math id="M6" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, aerosols have
relatively short lifetimes and hence large spatiotemporal variability
(Unger et al., 2008; Shindell et al., 2009). Therefore, the climatic and
health effects of aerosols are not only induced by inter-annual
concentration changes, but also strongly depend on their intra-annual
variability.</p>
      <?pagebreak page11248?><p id="d1e252"><?xmltex \hack{\newpage}?>Aerosol optical depth (AOD) has been widely used to represent the column
aerosol loading and to assess the aerosol impacts on radiation, clouds, and
precipitation (Ma et al., 2014; Niu and Li, 2012; Zhao et al., 2018b; Song et
al., 2017). However, the wide ranges of particle optical properties and size
distribution mean that even for the same AOD, different aerosol types have
different effects on not only the magnitude, but also the sign, of aerosol
radiative forcing (IPCC, 2013; Gu et al., 2006; Garrett et al., 2004).
IPCC (2013) estimate that the historical global mean direct radiative
forcings due to sulfate, organic carbon (OC), black carbon (BC), and mineral
dust are <inline-formula><mml:math id="M7" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.40</mml:mn></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M8" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.19</mml:mn></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M9" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.36</mml:mn></mml:mrow></mml:math></inline-formula>, and <inline-formula><mml:math id="M10" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.10</mml:mn></mml:mrow></mml:math></inline-formula> W m<inline-formula><mml:math id="M11" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, respectively.
Furthermore, absorbing and non-absorbing aerosols have been found to have
very different impacts on the surface radiative cooling effects (Yang et al.,
2016) and the development of convective clouds (Massie et al., 2016;
Ramanathan et al., 2005; Rosenfeld et al., 2008). Besides aerosol type, the
aerosol vertical distribution influences its mass concentration within the
planetary boundary layer (PBL) (Zheng et al., 2017) and the vertical profile
of heating rate (Johnson et al., 2008; Guan et al., 2010; Zhang et al.,
2013), which subsequently modifies the atmospheric stability and convective
strength (Ramanathan et al., 2007), with potential changes in cloud
properties (Johnson et al., 2004). Understanding aerosol variability as a
function of height is also important because the indirect effect of aerosols
is mainly dependent on those mixed with the clouds (Zhao et al., 2018c).
Meanwhile, the health impacts of aerosols are only associated with those
present near the surface, where they are inhaled. For these reasons,
systematic analyses of the intra-annual variations of aerosol vertical
distribution and particle types, in addition to total column AOD, are
necessary to improve our understanding of aerosol climatic and health
effects.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><caption><p id="d1e310">Target regions for this study: the Eastern United States (EUS),
Western Europe (WEU), and Eastern and Central China (ECC).</p></caption>
        <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/11247/2018/acp-18-11247-2018-f01.png"/>

      </fig>

      <p id="d1e319">Numerous studies have investigated the seasonal variations of AOD at global
and regional scales using satellite observations (e.g., Kim et al., 2007;
Song et al., 2009; Mehta et al., 2016; Mao et al., 2014). By comparison, most
previous studies of the temporal variations of aerosol vertical distributions
and aerosol types have been confined to only a few sites due to coverage
limitations associated with reliance on ground-based instruments (e.g., Liu
et al., 2012; Matthias et al., 2004). Despite continuous advancement of
remote sensing technology and emergence of new spaceborne sensors, only a
limited number of studies have utilized satellite observations to examine the
seasonal variations of aerosol profiles and/or types at regional or larger
scales (Huang et al., 2013; Kahn and Gaitley, 2015; Yu et al., 2010; Li et
al., 2016). Huang et al. (2013) analyzed the seasonal variations of aerosol
extinction profile and type distribution using 5-year observations from the
Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO).
Kahn and Gaitley (2015) examined the spatiotemporal variations of aerosol
types retrieved by the Multi-angle Imaging SpectroRadiometer (MISR).
Different satellite-borne sensors, such as MISR, CALIPSO, and the Moderate
resolution Imaging Spectroradiometer (MODIS), employ different principles of
measurement and retrieval, and thus provide different sensitivities to
column AOD, aerosol types, and vertical profiles. Therefore, integration of
data from multiple satellites and ground-based observational networks makes
it possible to deepen our understanding of the intra-annual variations of
aerosol loadings, profiles, and types.</p>
      <p id="d1e323">In this study, we investigate the seasonal variations of aerosol column
loading, vertical distribution, and particle types using multiple satellite
and ground-based observational datasets covering the period from 2007 to
2016. The purpose is to assess the consistency among various datasets and
provide a comprehensive characterization of aerosol properties in polluted
regions to facilitate future studies of aerosol climate effects and local air
quality issues. The data are from MISR, MODIS, CALIPSO, Aerosol Robotic
Network (AERONET), and surface PM<inline-formula><mml:math id="M12" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> monitors. Following our previous
study (Zhao et al., 2017), we selected three populous regions that have
experienced substantial anthropogenic pollution (Wang et al., 2017, 2014) and
have received considerable attention in other climate studies: the Eastern
United States (EUS; 29–45<inline-formula><mml:math id="M13" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 70–98<inline-formula><mml:math id="M14" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W), Western Europe
(WEU; 37–59<inline-formula><mml:math id="M15" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 10<inline-formula><mml:math id="M16" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W–17<inline-formula><mml:math id="M17" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E), and Eastern and
Central China (ECC; 21–41<inline-formula><mml:math id="M18" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 102–122<inline-formula><mml:math id="M19" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E). The
geographical boundaries of these regions are shown in Fig. 1.</p>
</sec>
<sec id="Ch1.S2">
  <title>Data and methods</title>
<sec id="Ch1.S2.SS1">
  <title>Satellite data</title>
      <p id="d1e410">We obtain retrievals of total column AOD as well as AOD for various height
ranges and aerosol types during 2007–2016 from MISR (flying on the Terra
satellite), MODIS (Terra and Aqua), and the Cloud-Aerosol Lidar with
Orthogonal Polarization (CALIOP) on CALIPSO. The aerosol retrievals from MISR
and MODIS are only available for clear-sky conditions in the daytime. CALIPSO
provides retrievals during both day and night, but only clear-sky daytime
profiles are used in order to be consistent with the products from MISR and
MODIS.</p>
      <?pagebreak page11249?><p id="d1e413">MISR observes the Earth with moderately high spatial resolution (275 m to
1.1 km) at nine along-track viewing angles in each of four visible or near-infrared
spectral bands, which enables the partitioning of AOD by particle type over
both land and ocean, in addition to retrieval of total AOD (Kahn and Gaitley,
2015; Kahn et al., 2001). Its observations provide near-global coverage every
9 days (Diner et al., 1998). We make use of the Level 3 daily global aerosol
product (MIL3DAE) version F15_0031, which is generated at a spatial
resolution of 0.5<inline-formula><mml:math id="M20" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M21" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.5<inline-formula><mml:math id="M22" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> based on the Level 2
aerosol product V22. The variables used in the analysis are total AOD at
555 nm as well as AODs for six aerosol components, namely small (<inline-formula><mml:math id="M23" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.7</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M24" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter), medium (0.7–1.4 <inline-formula><mml:math id="M25" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter), large
(<inline-formula><mml:math id="M26" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">1.4</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M27" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter), spherical, non-spherical, and absorbing.
Based on comparison with ground-based AERONET measurements, the errors in
MISR Level 2 AOD data are in the order of <inline-formula><mml:math id="M28" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.05</mml:mn></mml:mrow></mml:math></inline-formula> or <inline-formula><mml:math id="M29" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mo>(</mml:mo><mml:mn mathvariant="normal">0.20</mml:mn><mml:mo>×</mml:mo><mml:mi mathvariant="normal">AOD</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, whichever is larger (Kahn et al., 2005, 2010). In addition,
retrieval of MISR aerosol type information from individual retrievals is
considered to be reliable when <inline-formula><mml:math id="M30" display="inline"><mml:mrow><mml:mi mathvariant="normal">AOD</mml:mi><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">0.15</mml:mn></mml:mrow></mml:math></inline-formula>, and has diminished
sensitivity at smaller AOD (Kahn and Gaitley, 2015; Kahn et al., 2010). In
this study we use only monthly mean values, for which the uncertainties in
aerosol types are expected to be smaller than those for individual
retrievals. Note that we did not do a relative humidity (RH) correction to
AOD retrievals from MISR as well as other sensors. The seasonal variations of
AOD represent a combined effect of variations in aerosol abundance, vertical
distribution, chemical constituents, and meteorological conditions.</p>
      <p id="d1e523">The MODIS sensors onboard the Terra and Aqua satellites observe the Earth
with multiple wavelength bands over a 2330 km swath (King et al., 2003),
which provides near-daily global coverage. In this study we obtain column AOD
data at 550 nm with a 1<inline-formula><mml:math id="M31" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M32" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1<inline-formula><mml:math id="M33" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> resolution from the
Level 3 daily atmosphere products Collection 6 (MOD08 and MYD08 for the Terra
and Aqua platforms, respectively). Comparison studies with AERONET have
estimated the accuracy of Level 2 AOD retrievals to be about <inline-formula><mml:math id="M34" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mo>(</mml:mo><mml:mn mathvariant="normal">0.05</mml:mn><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.15</mml:mn><mml:mo>×</mml:mo><mml:mi mathvariant="normal">AOD</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> over land and <inline-formula><mml:math id="M35" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mo>(</mml:mo><mml:mn mathvariant="normal">0.03</mml:mn><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.05</mml:mn><mml:mo>×</mml:mo><mml:mi mathvariant="normal">AOD</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> over ocean (Levy et al., 2010; Remer et al., 2005). For both
MISR and MODIS data, we calculate regional mean AOD by averaging valid AOD
values over all grids within the three target regions.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><caption><p id="d1e598">Summary of the seasonal variations of the total, height-specific,
and type-specific AOD.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="4">
     <oasis:colspec colnum="1" colname="col1" align="justify" colwidth="99.584646pt"/>
     <oasis:colspec colnum="2" colname="col2" align="justify" colwidth="99.584646pt"/>
     <oasis:colspec colnum="3" colname="col3" align="justify" colwidth="99.584646pt"/>
     <oasis:colspec colnum="4" colname="col4" align="justify" colwidth="99.584646pt"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">EUS</oasis:entry>
         <oasis:entry colname="col3">WEU</oasis:entry>
         <oasis:entry colname="col4">ECC</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Total column AOD</oasis:entry>
         <oasis:entry colname="col2">Peak in summer</oasis:entry>
         <oasis:entry colname="col3">Peak in summer/late spring</oasis:entry>
         <oasis:entry colname="col4">Peak in summer/spring</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M36" display="inline"><mml:mrow><mml:mi mathvariant="normal">AOD</mml:mi><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">800</mml:mn></mml:mrow></mml:math></inline-formula> m a.g.l.</oasis:entry>
         <oasis:entry colname="col2">Peak in summer</oasis:entry>
         <oasis:entry colname="col3">Peak in summer/late spring</oasis:entry>
         <oasis:entry colname="col4">Peak in summer/spring</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M37" display="inline"><mml:mrow><mml:mi mathvariant="normal">AOD</mml:mi><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">800</mml:mn></mml:mrow></mml:math></inline-formula> m a.g.l.</oasis:entry>
         <oasis:entry colname="col2">Two peaks in winter and summer</oasis:entry>
         <oasis:entry colname="col3">Peak in winter</oasis:entry>
         <oasis:entry colname="col4">Peak in winter</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Small-size</oasis:entry>
         <oasis:entry colname="col2">Peak in summer</oasis:entry>
         <oasis:entry colname="col3">Peak in summer/late spring</oasis:entry>
         <oasis:entry colname="col4">Peak in summer/spring</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Medium-size</oasis:entry>
         <oasis:entry colname="col2">Peak in summer</oasis:entry>
         <oasis:entry colname="col3">Peak in summer/late spring</oasis:entry>
         <oasis:entry colname="col4">Peak in summer/spring</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Large-size</oasis:entry>
         <oasis:entry colname="col2">Rather uniform</oasis:entry>
         <oasis:entry colname="col3">Rather uniform</oasis:entry>
         <oasis:entry colname="col4">Peak in spring</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Absorbing</oasis:entry>
         <oasis:entry colname="col2">Peak in summer</oasis:entry>
         <oasis:entry colname="col3">Peak in summer/late spring</oasis:entry>
         <oasis:entry colname="col4">Two peaks in Mar and Aug</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Polluted continental dust</oasis:entry>
         <oasis:entry colname="col2">Similar to height-specific total AOD</oasis:entry>
         <oasis:entry colname="col3">Similar to height-specific total AOD</oasis:entry>
         <oasis:entry colname="col4">Similar to height-specific total AOD</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Dust</oasis:entry>
         <oasis:entry colname="col2">No obvious seasonal pattern</oasis:entry>
         <oasis:entry colname="col3">Peak in summer</oasis:entry>
         <oasis:entry colname="col4">Peak in spring</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Clean marine</oasis:entry>
         <oasis:entry colname="col2">No obvious seasonal pattern</oasis:entry>
         <oasis:entry colname="col3">Peak in winter</oasis:entry>
         <oasis:entry colname="col4">Negligible amount</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Smoke</oasis:entry>
         <oasis:entry colname="col2">Peak in summer</oasis:entry>
         <oasis:entry colname="col3">Peak in summer/late spring</oasis:entry>
         <oasis:entry colname="col4">Two peaks in Mar and Aug</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d1e824">CALIOP is a dual-wavelength polarization lidar on the CALIPSO satellite, and
is designed to acquire vertical profiles of aerosols and clouds at 532 and
1064 nm wavelengths (Winker et al., 2007). CALIPSO flies in formation with
Aqua, and all three satellites employed in this paper fly in orbits that have
16-day repeat cycles. In addition to vertical extinction profiles, CALIPSO
categorizes an aerosol layer as one of seven types based on a number of
parameters including altitude, location, surface type, volume depolarization
ratio, and integrated attenuated backscatter (Omar et al., 2009). The seven
aerosol types are dust, smoke, clean continental, polluted continental,
polluted dust, clean marine, and dusty marine. For most profiles, this
aerosol classification is consistent with that derived from AERONET inversion
data (Mielonen et al., 2009). In this study, we adopt the Level 2 aerosol
profile product (05kmAPro, V4.10), which has an along-track horizontal
resolution of 5 km and a vertical resolution of 60 m or 180 m, depending
on whether the aerosol height is below or above 20.2 km altitude. We do not
use the CALIOP Level 3 product because it is difficult to collocate with
AERONET observations (see Sect. 2.2) due to its coarse resolution
(<inline-formula><mml:math id="M38" display="inline"><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">5</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula>). For each clear-sky profile, we calculate
the column AOD at 532 nm by vertically integrating extinction coefficients
of the features that are identified as “aerosols” and have valid quality
control (QC) flags, i.e., <inline-formula><mml:math id="M39" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">100</mml:mn><mml:mo>≤</mml:mo></mml:mrow></mml:math></inline-formula> cloud aerosol discrimination (CAD)
score <inline-formula><mml:math id="M40" display="inline"><mml:mrow><mml:mo>≤</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">20</mml:mn></mml:mrow></mml:math></inline-formula>, extinction <inline-formula><mml:math id="M41" display="inline"><mml:mrow><mml:mi mathvariant="normal">QC</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>/</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>, and extinction coefficient
uncertainty <inline-formula><mml:math id="M42" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">99.9</mml:mn></mml:mrow></mml:math></inline-formula> (Huang et al., 2013). In addition, we employ two quality
filters used in generating the Level 3 product in order to eliminate features
that probably suffer from surface contamination, i.e., near-surface features
with large negative extinction coefficients and contaminated features beneath
the surface-attached opaque layer (NASA CALIPSO team, 2011). Following the
same method, we also bin the 532 nm AODs into various height ranges, i.e.,
0–200, 200–500, 500–800, 800–1200, 1200–2000, and <inline-formula><mml:math id="M43" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">2000</mml:mn></mml:mrow></mml:math></inline-formula> m above
ground level (a.g.l.). Finally, we derive monthly mean AODs by averaging all
clear-sky aerosol profiles within each month over the three target regions.
Although aerosol extinction coefficients with heights below 200 m a.g.l.
are considered to be uncertain despite the application of quality filters
(NASA<?pagebreak page11250?> CALIPSO team, 2011), we include them for completeness but exercise with
caution when interpreting variations of AODs below 200 m. It should be noted
that CALIPSO AOD is reported at a different wavelength (532 nm) from those
used in the MISR and MODIS products (555 and 550 nm, respectively); this
slight wavelength difference is not expected to affect our conclusions
regarding AOD seasonal variations.</p>
</sec>
<sec id="Ch1.S2.SS2">
  <?xmltex \opttitle{AERONET and surface PM${}_{{2.5}}$ data}?><title>AERONET and surface PM<inline-formula><mml:math id="M44" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> data</title>
      <p id="d1e924">We use AOD observations from AERONET to compare with the AOD seasonal
variations derived from satellite datasets. AERONET sunphotometers directly
measure AOD at seven wavelengths (approximately 340, 380, 440, 500, 675, 870,
and 1020 nm) with an estimated uncertainty of 0.01–0.02 (Holben et al.,
2001; Eck et al., 1999), which is much smaller than the uncertainties
associated with satellite measurements (Kahn et al., 2010; Levy et al., 2010;
Schuster et al., 2012). Therefore, we consider AERONET as “ground truth”
for AOD temporal variations. We adopt the AERONET Level 2 Version 2.0
direct-sun measurements of spectral AODs, which are subsequently interpolated
to 550 nm using a second-order polynomial fit to ln(AOD) vs. ln(wavelength)
as recommended by Eck et al. (1999). A fundamental difference between
satellite and AERONET AOD observations is that a satellite acquires data at a
single overpass time (or spread over 7 min for MISR's nine views) and over
an extended spatial area in the case of MISR and MODIS, whereas AERONET
obtains a time series of point data at each surface station. To match
coincident measurements, the AERONET AOD retrievals for each site are
averaged within a 2 h window centered on the satellite overpass times (about
10:30 for MISR and MODIS/Terra, and 13:30 for MODIS/Aqua and CALIPSO,
depending on site location), and compared with the satellite AOD retrievals
in a <inline-formula><mml:math id="M45" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> grid box (consistent with the grids used
in the MODIS Level 3 products) that contains the corresponding AERONET site.
Only those days for which a satellite overpasses an AERONET site are used in
the comparisons. As AOD variation has a large spatial correlation length
of 40–400 km (Anderson et al., 2003), spatial averaging over a <inline-formula><mml:math id="M46" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> grid should not bias the seasonal variations of AOD but
has the benefit of increase the number of data points with valid AOD
retrievals that are used in the comparisons. To assure data quality, only the
AERONET sites that span at least 5 years with at least 10 months of valid
data in each year are included in the comparison. After screening, 28, 54,
and 13 sites are used in our analysis of the EUS, WEU, and ECC regions.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2" specific-use="star"><caption><p id="d1e969">Monthly mean AOD observed by MISR, MODIS/Terra, MODIS/Aqua, and
CALIPSO during 2007–2016 in <bold>(a)</bold> EUS, <bold>(b)</bold> WEU, and
<bold>(c)</bold> ECC. For CALIPSO, only clear-sky daytime profiles are averaged
in order to be consistent with the MISR and MODIS products.
“MODIS/Terra_match MISR” is a sensitivity case in which the monthly mean
AOD of MODIS/Terra is calculated using only the days when MISR overpasses,
and “MODIS/Aqua_match CALIPSO” is a case in which the monthly mean AOD
of MODIS/Aqua is calculated using only the overpassing days of CALIPSO. The
error bars denote the standard deviation of the monthly mean AOD values
obtained over all years. Note the different scales on the <inline-formula><mml:math id="M47" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axes of the
plots.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/11247/2018/acp-18-11247-2018-f02.pdf"/>

        </fig>

      <?pagebreak page11251?><p id="d1e994">To provide additional information on the seasonal variations of
satellite-observed aerosol loadings near the surface, we obtain surface
PM<inline-formula><mml:math id="M48" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations from several observational networks over the three
target regions. Hourly PM<inline-formula><mml:math id="M49" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations for 225 sites over the EUS
region are achieved from the Air Quality System (AQS), which is a large
observational database containing ambient air pollution data collected by the
United States Environmental Protection Agency (USEPA), as well as state,
local, and tribal air pollution control agencies in the United States (USEPA,
2015). For the ECC region, we obtain hourly PM<inline-formula><mml:math id="M50" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations from
the Ministry of Environmental Protection of China (MEP,
<uri>http://datacenter.mep.gov.cn/</uri>, last access: 15 August 2017), which
provides continuous measurements at 496 sites located in 74 major cities in
China. Hourly and daily PM<inline-formula><mml:math id="M51" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations for 52 sites over the WEU
region are taken from the European Monitoring and Evaluation Programme
(EMEP). Similar to the processing of AERONET data, we only include sites
whose data span <inline-formula><mml:math id="M52" display="inline"><mml:mrow><mml:mo>≥</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> years with <inline-formula><mml:math id="M53" display="inline"><mml:mrow><mml:mo>≥</mml:mo><mml:mn mathvariant="normal">10</mml:mn></mml:mrow></mml:math></inline-formula> months of data in each year,
except in the case of the ECC region where at least 2 years of data are
required because the PM<inline-formula><mml:math id="M54" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations have been only publicly
available since January 2013.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <title>Results and discussion</title>
<sec id="Ch1.S3.SS1">
  <title>Seasonal variations of column AOD</title>
      <p id="d1e1078">Figure 2 illustrates the monthly variations in column AOD observed by MISR,
MODIS/Terra, MODIS/Aqua, and CALIPSO during 2007–2016 in the three target
regions. All satellite-borne sensors show that AOD in the EUS region is the
highest in summer and lowest in winter, though CALIPSO reports a noticeably
smaller difference between the summer and winter extrema compared with the
other three satellite instruments. For the WEU and ECC regions, MISR,
MODIS/Terra, and MODIS/Aqua also reveal consistent seasonal patterns in which
AOD peaks in spring and/or summer and reaches its lowest valley in winter.
However, CALIPSO shows little intra-annual variation in AOD, with small
peaks occurring in spring and fall.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><caption><p id="d1e1083">Monthly mean AOD observed by satellites and AERONET averaged across
the AERONET sites during 2007–2016 in <bold>(a)</bold> EUS, <bold>(b)</bold> WEU,
and <bold>(c)</bold> ECC. The observations from MISR, MODIS/Terra, MODIS/Aqua,
and CALIPSO are averaged over <inline-formula><mml:math id="M55" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> grid boxes
containing the AERONET sites. The AERONET data are averaged within a 2 h
window centered on satellite overpass times. The numbers of AERONET sites
included in analysis are 28, 54, and 13, in the EUS, WEU, and ECC regions,
respectively. As the four sensors overpass a site in different days and
different times of day, we separately calculate the AERONET data matched to
each sensor (denoted by “AERONET-<inline-formula><mml:math id="M56" display="inline"><mml:mrow><mml:mi>x</mml:mi><mml:mi>x</mml:mi><mml:mi>x</mml:mi></mml:mrow></mml:math></inline-formula>”). The AERONET curves matched to
different sensors are close in EUS and WEU, partly because there are plenty
of sites in these two regions, and the discrepancy due to the sampling issue
is thus smoothed out. In contrast, there are only 13 AERONET sites in
ECC, so there exists larger discrepancy between the AERONET data matched to
different sensors. Note the different scales on the <inline-formula><mml:math id="M57" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axes of the plots.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/11247/2018/acp-18-11247-2018-f03.pdf"/>

        </fig>

      <p id="d1e1141">As described in Sect. 2.1, MODIS provides near-daily global coverage but MISR
and CALIPSO do not. As a result, the monthly mean AOD from different sensors
is calculated based on different sets of days, which might lead to
uncertainties in the estimation of monthly mean AOD (Colarco et al., 2014;
Wang and Zhao, 2017). To rule out the impact of spatiotemporal sampling on
seasonal variation patterns, we design two sensitivity cases: a
“MODIS/Terra_match MISR” case in which the monthly mean AOD of
MODIS/Terra is calculated using only the days when MISR overpasses, and a
“MODIS/Aqua_match CALIPSO” case in which the monthly mean AOD of
MODIS/Aqua is calculated using only the overpassing days of CALIPSO. The
results are illustrated in Fig. 2. In all three regions, the monthly mean
AODs are slightly different for “MODIS/Terra” and “MODIS/Terra_match
MISR”, but the seasonal variation patterns are largely the same. The same
results are found for “MODIS/Aqua” and “MODIS/Aqua_match CALIPSO”. As
such, we conclude that sampling has little effect on the AOD seasonal
variation patterns reported in this study. In fact, this conclusion is
compatible with the findings of Colarco et al. (2014). Colarco et al. (2014)
revealed that the spatial sampling artifacts were significant for fine
aggregation grid (e.g., 0.5<inline-formula><mml:math id="M58" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>), but they are reduced at coarse grid
scales (e.g., 10<inline-formula><mml:math id="M59" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>). In this study, we use only the mean AOD over
three large regions (about <inline-formula><mml:math id="M60" display="inline"><mml:mrow><mml:mn mathvariant="normal">20</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">20</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula>) across 10 years,
thus the sampling artifacts are expected to be even smaller. Despite this, we acknowledge that the inconsistent spatiotemporal sampling of
different retrieval products (due to different swath width and mixing of
Level 2 and Level 3 products) adds to the uncertainty in monthly AOD
estimation. A more direct comparison at the measurement/retrieval level
merits further in-depth study.</p>
      <p id="d1e1182">In view of the substantial differences between CALIPSO and the other three
sensors, we compare satellite retrieved AOD seasonal variations with
point-based ground measurements from AERONET (Fig. 3). As in other studies,
AERONET data are treated as “ground truth” for column AOD due to its
smaller uncertainty compared with satellite data (Kahn et al., 2010; Levy et
al., 2010; Schuster et al., 2012; Fan et al., 2018). Figure 3 shows that, in
all three regions, the AOD seasonal variations measured by AERONET are
similar to those retrieved by MISR, MODIS/Terra, and MODIS/Aqua, but are
quite different from CALIPSO data. Reasons for the different seasonal
patterns between CALIPSO and other sensors will be discussed in Sect. 3.2.
Considering the high accuracy of AERONET, we conclude that AOD peaks in
summer/spring and dips in winter. An important reason for the higher AOD in
summer is that the stronger radiation and higher temperature<?pagebreak page11252?> accelerate the
formation of secondary aerosols (Timonen et al., 2014), including sulfate,
nitrate, ammonium, and secondary organic aerosol (SOA). SOA is produced by
photo-oxidation of volatile organic compounds (VOCs) and intermediate
volatility organic compounds (IVOCs), as well as the chemical aging of
primary organic aerosol (Zhao et al., 2016). Another reason is that more
abundant water vapor in summer favors the hygroscopic growth of aerosols (Liu
et al., 2012; Zheng et al., 2017). The different patterns of long-range
transport as a function of season is also partly responsible for the
seasonable variation of AOD (Tian et al., 2017; Yang et al., 2018; Garrett et
al., 2010).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><caption><p id="d1e1188">Monthly mean AOD as a function of height above ground level observed
by CALIPSO during 2007–2016 in <bold>(a)</bold> EUS, <bold>(b)</bold> WEU, and
<bold>(c)</bold> ECC. Only clear-sky daytime profiles are averaged in order to be
consistent with the products of MISR and MODIS. The range of AOD within a
particular height range is depicted by the colored stacks. The integrated
AODs for heights below and above 800 m are shown as solid lines, for which
the error bars are defined in the same way as in Fig. 2. Note the different
scales on the <inline-formula><mml:math id="M61" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axes of the plots.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/11247/2018/acp-18-11247-2018-f04.pdf"/>

        </fig>

      <p id="d1e1213">While relative patterns of AOD seasonal variations from observations of MISR,
MODIS/Terra, and MODIS/Aqua are similar to each other and to those of
AERONET, the magnitude of AOD observed by these sensors shows considerable
discrepancies. In all three regions, the AOD retrieved from MODIS is larger
than that from MISR, consistent with the results of previous studies (de Meij
et al., 2012; Zhao et al., 2017; Chin et al., 2014; Kang et al., 2016; Qi et
al., 2013). This is most likely due to differences in observing strategy,
retrieval algorithms, and spatiotemporal sampling (Kahn et al., 2009). The
MISR-retrieved AOD agrees well with the AERONET observations in EUS and WEU
regions. However, in the ECC region MISR underestimates the AERONET AOD,
probably because there is less signal from the surface at higher AOD, which
creates ambiguity that can result in the algorithm assigning too much of the
top-of-atmosphere radiance to the surface (i.e., a higher surface albedo),
thereby underestimating the AOD (Kahn et al., 2010). The MODIS/Terra and
MODIS/Aqua overestimate the AERONET AOD to some extent in all three regions.
The overestimation was also reported in two previous studies (de Meij et al.,
2012; Ruiz-Arias et al., 2013) using the level 3 MODIS products (Collection 5
or 5.1). We show a relatively larger overestimation than that reported by de
Meij et al. (2012) and Ruiz-Arias et al. (2013), partly because we used the
AERONET AOD averaged within a 2 h window centered on the satellite overpass
times while the two previous studies used the daily/monthly mean AERONET AOD
in the comparisons. The daily mean AOD observed by AERONET is about 10 %
larger than the value during the satellite overpass times (Li et al., 2013).
The reasons for the discrepancy between MODIS and AERONET are yet to be
thoroughly investigated.</p>
</sec>
<sec id="Ch1.S3.SS2">
  <title>Seasonal variations of aerosol loadings as a function of height</title>
      <p id="d1e1222">In addition to column AOD, the climatic effects of aerosols are also strongly
dependent on their vertical distribution. To explore intra-annual variations
in aerosol vertical profile, Fig. 4 presents CALIPSO-observed monthly
variations of AOD as a function of height in the three target regions. A
striking pattern is that the AOD seasonal variations are dramatically
different at lower and upper heights. Over the WEU and ECC regions, AODs of
the vertical layers below 800 m a.g.l. generally peak in winter, while
those above 800 m a.g.l. peak in summer/spring. As a result, the
CALIPSO-observed column AOD for these two regions presents a rather uniform
seasonal pattern. For the EUS region, the maximum AOD above 800 m a.g.l.
also occurs in summer; however, AOD below 800 m a.g.l. shows two peaks, one
in summer and the other in winter. The integration of<?pagebreak page11253?> various layers thus
yields a nearly unimodal distribution with maximum occurring in summer.</p>
      <p id="d1e1225">To provide an independent evaluation of the CALIPSO-observed AOD variations
at lower heights, we examine the seasonal variations of near-surface
PM<inline-formula><mml:math id="M62" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations at hundreds of surface monitor locations within the
three target regions (Fig. 5). The aerosol extinction coefficient, and hence
AOD at lower heights is affected by not only the particle mass
concentrations, but also aerosol type (absorbing vs. non-absorbing aerosols,
coarse-mode vs. fine-mode aerosols) and meteorological parameters such as RH,
wind speed and direction, and planetary boundary layer height (Zheng et al.,
2017). Nevertheless, previous studies have reported fairly good correlations
between extinction coefficient/low-level AOD and PM<inline-formula><mml:math id="M63" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations
(Cheng et al., 2013; Zheng et al., 2017). For this reason, it is reasonable
to qualitatively compare the seasonal variation patterns of near-surface
PM<inline-formula><mml:math id="M64" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations and low-level AOD. We calculate monthly mean
PM<inline-formula><mml:math id="M65" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations using only the days when CALIPSO overpasses an
observational site to enable a better comparison. Figure 5 shows that, over
the ECC and WEU regions, surface PM<inline-formula><mml:math id="M66" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations are largest in
winter and smallest in summer. In the EUS region, the maximum PM<inline-formula><mml:math id="M67" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula>
concentration occurs in summer and a second maximum occurs in winter. These
trends are generally consistent with the seasonal variations of AOD at low
heights, implying that CALIPSO data can generally capture the seasonal
changes in low-level aerosol abundance.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><caption><p id="d1e1285">Monthly mean surface PM<inline-formula><mml:math id="M68" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations during 2007–2016 in
three target regions. The numbers of observational sites included in
averaging are 225, 52, and 496, in the EUS, WEU, and ECC regions. Note the
different scales on the <inline-formula><mml:math id="M69" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axes for EUS/WEU and ECC.</p></caption>
          <?xmltex \igopts{width=227.622047pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/11247/2018/acp-18-11247-2018-f05.pdf"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><caption><p id="d1e1313">Monthly mean AOD of different aerosol types observed by MISR during
2007–2016 in <bold>(a)</bold> EUS, <bold>(b)</bold> WEU, and <bold>(c)</bold> ECC. The
size-resolved AODs are depicted by the colored stacks (left <inline-formula><mml:math id="M70" display="inline"><mml:mi>Y</mml:mi></mml:math></inline-formula> axis); the
integration of the three size ranges yields total column AOD, as represented
by the upper edge of the blue color. The AOD of absorbing aerosols is shown
as solid lines (right <inline-formula><mml:math id="M71" display="inline"><mml:mi>Y</mml:mi></mml:math></inline-formula> axis), for which the error bars are defined in the
same way as in Fig. 2. Note the different scales on the <inline-formula><mml:math id="M72" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axes of the
plots.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/11247/2018/acp-18-11247-2018-f06.pdf"/>

        </fig>

      <p id="d1e1353">The aerosol vertical distribution is an important factor in reconciling
CALIPSO and other sensors with regard to AOD seasonal variations. MISR,
MODIS, and AERONET all measure column-integrated AOD using
spectroradiometers, whereas CALIOP is an active lidar which estimates
vertically resolved AOD based on vertical profiles of attenuated backscatter.
By comparing CALIPSO with the Atmospheric Radiation Measurement (ARM)
program's ground-based Raman lidars, Thorsen et al. (2017) showed that
CALIPSO does not detect all relatively significant aerosols due to
insufficient detection sensitivity and tends to miss optically thin aerosol
layers. Consequently, the fraction of aerosols detected in the upper levels
(<inline-formula><mml:math id="M73" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">800</mml:mn></mml:mrow></mml:math></inline-formula> m a.g.l.) is much smaller than that in the lower levels (<inline-formula><mml:math id="M74" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">800</mml:mn></mml:mrow></mml:math></inline-formula> m a.g.l.) because the upper-level aerosols are often optically thin.
As a result, the CALIPSO-observed AOD seasonal variations are significantly
weighted toward lower heights. Note that the aerosols with heights below
200 m a.g.l. are frequently undetected because of surface contamination
(Kim et al., 2017; NASA CALIPSO team, 2011), but this does not alter the key
feature that the AOD is weighted toward lower heights. Over WEU and ECC
regions, the unimodal AOD distributions with a summer peak at higher levels
are largely counteracted by the opposite seasonal variations at lower levels,
resulting in rather uniform seasonal variations of column AOD. For the EUS
regions, due to the bimodal AOD distribution at lower heights, the summer
peak in column AOD variations remain but the difference between peak and
valley is smaller than implied by<?pagebreak page11254?> the observations of MISR/MODIS/AERONET. In
this sense, although the integrated CALIPSO column AOD does not agree well
with AERONET, it does provide valuable information with respect to seasonal
variations of aerosols within a specific height range. This is because the
detection fraction of aerosols does not vary significantly with season at a
given height due to relatively small variability of optical thickness.
Specifically, the seasonal mean AOD within a specific height range differs by
3 times at most as a function of season (Fig. 4), while it decreases by about
2 orders of magnitude with the increase of height (Kim et al., 2017; Thorsen
et al., 2017). Aside from the seasonal variations, the difference in the
magnitude of AOD between CALIPSO and other sensors are also largely explained
by the undetected aerosol layers by CALIPSO (Kim et al., 2017; Thorsen et
al., 2017) as well as the assumed lidar ratios in CALIPSO retrievals (Ma et
al., 2013).</p>
      <p id="d1e1376">Why are the AOD seasonal variations different between the lower and upper
levels? The atmosphere in winter is generally more stable and vertical mixing
is weaker, thus more aerosols, particularly primary aerosols, are
confined to lower heights, resulting in the peak of low-level AOD in winter
(Guo et al., 2016; Liu et al., 2012; Zheng et al., 2017). At higher levels,
the maximum AOD in summer can be explained by two reasons: (1) more aerosols,
especially primary aerosols, are transported to the upper levels in summer
due to stronger vertical mixing (Guo et al., 2016; Liu et al., 2012; Zheng et
al., 2017), and (2) secondary aerosol formation is more rapid in summer
because of stronger radiation and higher temperature, and much of the
secondary aerosols are produced in the upper levels (de Reus et al., 2000;
Minguillon et al., 2015; Heald et al., 2005). In addition, the seasonal
variations of AOD at different vertical levels may also be influenced by the
variations of water vapor amount, which affects the hygroscopic growth (Liu et
al., 2012; Zheng et al., 2017) as well as the seasonal patterns of
inter-regional transport of aerosols (Tian et al., 2017; Yang et al., 2018;
Garrett et al., 2010).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><caption><p id="d1e1381">Monthly mean AOD of different aerosol types <bold>(a–c)</bold> below
800 m and <bold>(d–f)</bold> above 800 m observed by CALIPSO during 2007–2016
in <bold>(a, d)</bold> EUS, <bold>(b, e)</bold> WEU, and <bold>(c, f)</bold> ECC. Only
clear-sky daytime profiles are used in the averaging to be consistent with
the products of MISR and MODIS. The definition of error bars is the same as
in Fig. 2. Note the different scales on the <inline-formula><mml:math id="M75" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axes of the plots.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/11247/2018/acp-18-11247-2018-f07.pdf"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS3">
  <title>Seasonal variations of aerosol types</title>
      <p id="d1e1419">Aside from column AOD and vertical profiles, another factor influencing
aerosol climate impact is aerosol type (i.e., partitioning by size and
chemical composition). The MISR and CALIPSO products classify aerosols based
on distinct principles of measurement and retrieval algorithms. Analysis of
the two datasets in combination can potentially lead to a deeper
understanding of the factors driving temporal variations of aerosol type. Key
features of intra-annual variations of various aerosol types are summarized
in Table 1.</p>
      <p id="d1e1422">Figures 6 illustrates the seasonal variations of type-specific AODs retrieved
by MISR. MISR distributes AODs into three size ranges, i.e., small (<inline-formula><mml:math id="M76" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.7</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M77" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter), medium (0.7–1.4 <inline-formula><mml:math id="M78" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter), and
large (<inline-formula><mml:math id="M79" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">1.4</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M80" display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m diameter). The ambient aerosols are comprised of
primary aerosols (dust, sea-spray aerosols, and primary anthropogenic
aerosols) and secondary aerosols (sulfate, nitrate, ammonium, and SOA). Among
these constituents, dust and sea-spray aerosols are predominantly coarse
particles and secondary aerosols are dominated by very fine particles, while
primary anthropogenic aerosols span a large size range, leading to a mean
size intermediate between dust/sea-spray and secondary constituents (Seinfeld
and Pandis, 2006). Figure 6 indicates that the small-size AOD is much larger
in spring/summer than in winter over all regions, primarily due to
accelerated secondary aerosol formation and enhanced hygroscopic growth (see
Sect. 3.1). In contrast, large-size AOD generally shows rather uniform
distributions, except for the ECC region where a peak occurs in late
winter/early spring. AOD of primary anthropogenic aerosols are less
influenced by seasonal effects than secondary aerosols, which partly accounts
for the rather uniform distributions of large-size AOD. Additionally, the
seasonal variations of large-size AOD are also affected by dust and sea-spray
aerosols, as discussed below.</p>
      <p id="d1e1466">In contrast to MISR's partitioning of aerosol type by size and absorption,
the CALIPSO-retrieved aerosol types are<?pagebreak page11255?> characterized by emission source
(Fig. 7). As discussed in Sect. 3.2, relative variability in CALIPSO-derived
AOD at different height ranges appears to be more reliable than integrated
column AOD, thus we show aerosol types below and above 800 m separately
in Fig. 7. Particles associated with anthropogenic air pollution (polluted
continental and polluted dust) comprise the dominant type in all three
regions. The seasonal variation patterns of polluted continental/dust are in
accordance with those of the total AOD. Specifically, at higher levels, the
maximum AOD of polluted continental/dust aerosols occurs in spring/summer in
all regions. However, at lower levels the maximum occurs in winter (plus a
second maximum in summer in EUS).</p>
      <p id="d1e1469">With regard to dust and clean marine (sea-spray) aerosols, the AOD in the EUS
region does not show an obvious seasonal pattern. In the WEU region, AOD of
dust aerosols peaks in summer, consistent with previous surface-based
observational studies which show that dust events in Europe predominantly
occur during summer due to transport from the Sahara region (Stafoggia et
al., 2016). The AOD of dust is primarily located above 800 m, supporting the
conclusion that dust aerosols in WEU mainly originate from long range
transport. As the dust AOD is subject to a large inter-annual variability
(denoted by the large error bars in Fig. 7), we use the Student's <inline-formula><mml:math id="M81" display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula> test to
demonstrate the statistical significance of the seasonal variations. The dust
AOD in summer is statistically larger than that in any other season at the
0.05 level, indicating the robustness of the peak in summer. Contrary to
dust, the AOD of sea-spray aerosols in WEU is much higher in winter than in
summer, probably because winter is the relative windy season with large low
pressure systems over the Atlantic Ocean and the North Sea (Manders et al.,
2009). The offset of the opposite variation trends in dust and sea-spray
aerosols partly accounts for the rather uniform distributions of large-size
AOD in WEU (see Fig. 6). Over the ECC region, sea-spray aerosols make a
negligible contribution to total AOD. The dust AOD is much larger in spring
than in any other season (significant at the 0.05 level), which is tied to
the outburst of springtime Gobi desert dust storms (China Meteorological
Administration, 2012). The high dust AOD explains the peak in large-size AOD
in spring over the ECC region (see Fig. 6).</p>
      <?pagebreak page11256?><p id="d1e1480">Smoke aerosols are predominantly located above 800 m in all regions. Over the
EUS and WEU regions, smoke aerosols present a unimodal distribution with
maximum occurring in summer. The differences between smoke AOD in summer and
the other three seasons are all statistically significant at the 0.05 level,
except for the difference between summer and spring over the WEU region,
which is statistically significant at the 0.10 level. In the ECC region, the
smoke AOD follows a bimodal distribution with peaks occurring in March and
August and valleys occurring in May and December. The differences between
either of the peak months and either of the valley months are statistically
significant at the 0.05 level. MISR's independent retrieval of absorbing AOD
(Fig. 6) presents a highly similar seasonal pattern (statistically
significant at the 0.05 level) as the CALIPSO smoke AOD. In fact, smoke and
absorbing aerosols are closely correlated with each other, as smoke
consists of a much larger fraction of absorbing aerosols (Dubovik et al.,
2002), such as BC and light-absorbing organic aerosol (Kirchstetter and
Thatcher, 2012), as compared to other aerosol types. Besides, the MISR
absorbing AOD and CALIPSO smoke AOD are also consistent in the order of
magnitude. The variability of MISR absorbing AOD (shown in the right <inline-formula><mml:math id="M82" display="inline"><mml:mi>Y</mml:mi></mml:math></inline-formula> axis
of Fig. 6) is about 0.002–0.005, while the variability of smoke AOD from
CALIPSO is about 0.01–0.03. The smoke AOD includes the contributions of both
the absorbing and scattering portions. The MISR absorbing AOD, which is
calculated using total <inline-formula><mml:math id="M83" display="inline"><mml:mrow><mml:mi mathvariant="normal">AOD</mml:mi><mml:mo>×</mml:mo></mml:mrow></mml:math></inline-formula> (1 <inline-formula><mml:math id="M84" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula> single scattering
albedo), represents only the absorbing portion but includes contributions
from aerosol types other than smoke (Bull et al., 2011). Considering that the
single scattering albedo of smoke is about 0.80–0.94 (Dubovik et al., 2002),
we are able to reconcile the magnitude of MISR absorbing AOD and CALIPSO
smoke AOD. For the preceding reasons, the seasonal patterns of smoke and
absorbing aerosols act as a cross-validation and strengthen the reliability
of the observed trends. Over the EUS and WEU regions, the largest smoke AOD
in summer could be explained by the highest emissions from forest and
grassland fires (van der Werf et al., 2017). Over the ECC region, an
additional peak occurs in March because agricultural residue burning makes a
substantial contribution to total smoke emissions (van der Werf et al.,
2017), and such burning takes place more frequently in March due to burning
of crop residues left on the fields from the previous growing season (Shon,
2015).</p>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <title>Conclusions and implications</title>
      <p id="d1e1514">This study investigated the seasonal variations of aerosol column loading,
vertical distribution, and particle types using multiple satellite and
ground-based observational datasets during 2007–2016 over EUS, WEU, and ECC
regions. Retrievals from MISR and MODIS reveal that column AOD in all three
regions peaks in spring/summer and reaches its low in winter, which is
consistent with observations from AERONET. This seasonal pattern is probably
explained by accelerated formation of secondary aerosols in spring/summer due
to stronger insolation and higher temperature. In contrast, CALIPSO shows a
much weaker seasonal variability in column AOD, probably because
CALIPSO-retrieved AOD is weighted toward lower heights, as some thin
aerosol layers in high levels are undetected due to insufficient detection
sensitivity. Despite the discrepancy in integrated column AOD, CALIPSO does
provide valuable information with respect to intra-annual variations of AOD
as a function of height. Over the WEU and ECC regions, AODs of the vertical
layers below 800 m generally peak in winter, while those above 800 m mostly
peak in summer. For the EUS region, the maximum AOD above 800 m also occurs
in summer; however, AOD below 800 m shows two peaks, one in summer and the
other in winter. The seasonal variations of AOD at low heights are consistent
with seasonal patterns of measured surface PM<inline-formula><mml:math id="M85" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations.</p>
      <p id="d1e1526">When aerosols are binned into different size ranges, the small-size AOD is
much larger in spring/summer than in winter over all three regions.
Large-size AOD generally shows rather uniform distributions, except for the
ECC region where a peak occurs in spring, consistent with the largest dust
AOD in this season. When aerosols are classified according to sources, the
aerosols associated with anthropogenic air pollution (as well as mixtures of
anthropogenic pollution and dust) are the dominant type in all three regions.
AOD of polluted aerosols has a similar seasonal pattern as total AOD. Dust
and clean marine aerosols in the WEU region peak in summer and winter,
respectively, whereas they do not show an obvious seasonal pattern in the EUS
region. Smoke aerosols, which CALIPSO indicates are predominantly located at
heights above 800 m, present an obvious unimodal distribution with maximum
occurring in summer over EUS and WEU regions, and a bimodal distribution with
peaks in August and March over the ECC region. This pattern is in good
agreement with the seasonal variations of absorbing AOD derived from MISR.</p>
      <p id="d1e1529">The combination of multiple satellite and ground-based observations
facilitate a systematic and deeper understanding of the seasonal variations
of aerosols, particularly their vertical and type distribution. Comparison of
multiple measurement and retrieval methodologies enables reducing the
uncertainties in the estimation of aerosol direct effects by providing
improved information about aerosol vertical and type distributions, which
significantly affect the aerosol-induced scattering and absorption of
radiation. More importantly, the intra-annual variations of vertical
distributions and types of aerosols are important for understanding their
impact on atmospheric dynamics, cloud fields, and precipitation production
(Ramanathan et al., 2005; Massie et al., 2016; Zhao et al., 2018a; Wang et
al., 2013). Finally, the data and variation patterns presented in this study
can be used to evaluate and improve model simulations, with the ultimate goal
of improving model assessment of the climatic and health effects of aerosols.</p>
</sec>

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

      <p id="d1e1537">The data needed to evaluate the results and conclusions
have been presented in the text and figures. Additional related data will be
available upon request.</p>
  </notes><notes notes-type="authorcontribution">

      <p id="d1e1543">JHJ and BZ designed the research; BZ, JHJ, YG, ZJ, LH, and
YT conducted the research; BZ, JHJ, DJD, HS, YG, KNL, ZJ, XF, and AHO analyzed
the results; BZ, JHJ, and YG wrote the paper with contributions from all
coauthors.</p>
  </notes><notes notes-type="competinginterests">

      <p id="d1e1549">The authors declare that they have no conflict of
interest.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e1555">This study was supported by the MISR project at the Jet Propulsion
Laboratory, California Institute of Technology, under contract with NASA,
NASA CCST and TASNPP (Grant 80NSSC18K0985) programs, and NSF AGS-1701526. We
acknowledge Michael J. Garay and Jason L. Tackett for their valuable comments
and suggestions.<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?> Edited by: Xiaohong
Liu<?xmltex \hack{\newline}?> Reviewed by: two anonymous referees</p></ack><ref-list>
    <title>References</title>

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    <!--<article-title-html>Intra-annual variations of regional aerosol optical depth, vertical distribution, and particle types from multiple satellite and ground-based observational datasets</article-title-html>
<abstract-html><p>The climatic and health effects of aerosols are strongly dependent on the
intra-annual variations in their loading and properties. While the seasonal
variations of regional aerosol optical depth (AOD) have been extensively
studied, understanding the temporal variations in aerosol vertical
distribution and particle types is also important for an accurate estimate of
aerosol climatic effects. In this paper, we combine the observations from
four satellite-borne sensors and several ground-based networks to investigate
the seasonal variations of aerosol column loading, vertical distribution, and
particle types over three populous regions: the Eastern United States (EUS),
Western Europe (WEU), and Eastern and Central China (ECC). In all three
regions, column AOD, as well as AOD at heights above 800&thinsp;m, peaks in
summer/spring, probably due to accelerated formation of secondary aerosols
and hygroscopic growth. In contrast, AOD below 800&thinsp;m peaks in winter over
WEU and ECC regions because more aerosols are confined to lower heights due
to the weaker vertical mixing. In the EUS region, AOD below 800&thinsp;m shows two
maximums, one in summer and the other in winter. The temporal trends in
low-level AOD are consistent with those in surface fine particle
(PM<sub>2.5</sub>) concentrations. AOD due
to fine particles ( &lt; 0.7&thinsp;µm diameter) is much larger in
spring/summer than in winter over all three regions. However, the coarse mode
AOD ( &gt; 1.4&thinsp;µm diameter), generally shows small variability,
except that a peak occurs in spring in the ECC region due to the prevalence
of airborne dust during this season. When aerosols are classified according
to sources, the dominant type is associated with anthropogenic air pollution,
which has a similar seasonal pattern as total AOD. Dust and sea-spray
aerosols in the WEU region peak in summer and winter, respectively, but do
not show an obvious seasonal pattern in the EUS region. Smoke aerosols, as
well as absorbing aerosols, present an obvious unimodal distribution with a
maximum occurring in summer over the EUS and WEU regions, whereas they follow
a bimodal distribution with peaks in August and March (due to crop residue
burning) over the ECC region.</p></abstract-html>
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