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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-22-9949-2022</article-id><title-group><article-title>Arctic spring and summertime aerosol optical depth baseline from long-term
observations and model reanalyses – Part 2: Statistics of extreme AOD
events, and implications for the impact of regional biomass burning
processes</article-title><alt-title>Arctic spring and summertime AOD baseline – Part 2</alt-title>
      </title-group><?xmltex \runningtitle{Arctic spring and summertime AOD baseline -- Part 2}?><?xmltex \runningauthor{P.~Xian et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Xian</surname><given-names>Peng</given-names></name>
          <email>peng.xian@nrlmry.navy.mil</email>
        <ext-link>https://orcid.org/0000-0002-9661-8045</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Zhang</surname><given-names>Jianglong</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-8647-3519</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>O'Neill</surname><given-names>Norm T.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Reid</surname><given-names>Jeffrey S.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Toth</surname><given-names>Travis D.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Sorenson</surname><given-names>Blake</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-1727-9012</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Hyer</surname><given-names>Edward J.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-8636-2026</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Campbell</surname><given-names>James R.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-0251-4550</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3 aff5">
          <name><surname>Ranjbar</surname><given-names>Keyvan</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-2328-1963</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Naval Research Laboratory, Monterey, CA, USA</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Department of Atmospheric Sciences, University of North Dakota, Grand
Forks, ND, USA</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Département de géomatique appliqué, Université de
Sherbrooke, Sherbrooke, Quebec, Canada</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>NASA Langley Research Center, Hampton, Virginia, USA</institution>
        </aff>
        <aff id="aff5"><label>a</label><institution>now at: Flight Research Laboratory, National Research Council Canada,
Ottawa, ON, Canada</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Peng Xian (peng.xian@nrlmry.navy.mil)</corresp></author-notes><pub-date><day>3</day><month>August</month><year>2022</year></pub-date>
      
      <volume>22</volume>
      <issue>15</issue>
      <fpage>9949</fpage><lpage>9967</lpage>
      <history>
        <date date-type="received"><day>30</day><month>September</month><year>2021</year></date>
           <date date-type="rev-request"><day>3</day><month>November</month><year>2021</year></date>
           <date date-type="rev-recd"><day>16</day><month>May</month><year>2022</year></date>
           <date date-type="accepted"><day>27</day><month>May</month><year>2022</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2022 </copyright-statement>
        <copyright-year>2022</copyright-year>
      <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><title>Abstract</title>

      <p id="d1e183">In a companion paper (Xian et al., 2022, part 1 of the study), we present an Arctic aerosol
optical depth (AOD) climatology and trend analysis for 2003–2019 spring and
summertime periods derived from a combination of aerosol reanalyses, remote-sensing retrievals, and ground observations. Continued from the previous
discussion and as the second part of the study, we report the statistics and
trends of Arctic AOD extreme events using the U.S. Navy Aerosol Analysis and
Prediction System ReAnalysis version 1 (NAAPS-RA v1), the sun photometer
data from the AErosol RObotic NETwork (AERONET) sites, and the oceanic
Maritime Aerosol Network (MAN) measurements. Here, extreme AOD events are
defined as events with AOD exceeding the 95th percentile (denoted
“AOD<inline-formula><mml:math id="M1" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula>”) of AOD distributions for given locations using 6-hourly or
daily AOD data. While AERONET and MAN data estimate the Arctic median
550 nm AOD value to be 0.07, the 95th percentile value is 0.24. Such extreme
events are dominated by fine-mode aerosol particles, largely attributable to
biomass burning (BB) smoke events for the North American Arctic, the Asian
Arctic, and most areas of the Arctic Ocean. However, extreme AOD events for
the lower European Arctic are more attributable to anthropogenic and biogenic fine
particles. The extreme-event occurrence dominance of sea salt is largely
limited to the North Atlantic and Norwegian Sea. The extreme AOD amplitudes
of anthropogenic and biogenic fine-mode and sea salt AOD are, however,
significantly lower than those regions where extreme smoke AOD is dominant.
Even for sites distant from BB source regions, BB smoke is the principal
driver of AOD variation above the AOD<inline-formula><mml:math id="M2" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> threshold.</p>

      <p id="d1e204">Maximum AOD values in the high Arctic in 2010–2019 have increased compared
to 2003–2009, indicating stronger extreme BB smoke influence in more recent
years. The occurrence of extreme smoke events tended to be more equally
distributed over all months (April–August) during the 2003–2009 period while
being more concentrated in the late season (July–August) during the
2010–2019 period. The temporal shift of the occurrence of AOD extreme events
is likely due to improved control of early-season agriculture burning,
climate-change-related increases in summertime lightning frequencies, and a
reduction in anthropogenic pollution over the 2010–2019 period.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e216">Warming faster than the rest of the world, the Arctic is a focal point for
global warming (Serreze and Francis, 2006; Serreze and Barry, 2011).
Interactions between the atmosphere, ocean, land surface, and sea ice,
compounded by numerous human factors make the Arctic climate system
challenging to predict, with large diversity between current numerical model
outcomes (IPCC, 2021). Aerosol particles from anthropogenic and natural
sources affect regional energy balance through direct radiative processes
and indirect cloud processes (Quinn et al., 2008;
Flanner, 2013; Sand et al., 2013; Markowicz et al., 2021; Yang et al.,
2018). When deposited on the surface of snow and ice, light-absorbing
aerosol particles, including dust and <?xmltex \hack{\mbox\bgroup}?>black/brown<?xmltex \hack{\egroup}?> carbon from biomass
burning and anthropogenic emissions, can trigger albedo feedbacks and
accelerate melting (Hansen and Nazarenko, 2004; Jacobson, 2004; Flanner et
al., 2007; Skiles et al., 2018; Dang et al., 2017; Kang et al., 2020).</p>
      <p id="d1e223">Arctic aerosol concentrations are in general relatively low, with spring and
summertime median/mean 550 nm aerosol optical depths (AODs) of 0.06–0.07
(e.g., Tomasi et al., 2007; Saha et al., 2010; AboEl-Fetouh et al., 2020) as
compared to a global mean of roughly 0.20 over land and 0.12 over water
(e.g., Levy et al., 2010; Lynch et al., 2016; Schutgens et al., 2020;
Sogacheva et al., 2020). Extreme AOD events do occur within the Arctic,
mostly associated with large-scale transport from lower latitudes. Biomass
burning (BB) smoke from boreal wildfires, for example, can episodically
result in record-high Arctic AOD (Lund Myhre et al., 2007; Stohl et al., 2007;
Markowicz et al., 2016; Ranjbar et al., 2019). Some strong smoke events were
recorded during intensive field campaigns, including the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) and the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) campaigns in the summer of 2008 (Matsui et al., 2011; Saha et al., 2010;
McNaughton et al., 2011). More extreme BB smoke
cases in the Arctic can be found in Sect. 3.3.</p>
      <p id="d1e226">Extreme AOD events cause large perturbations in regional energy balance
(e.g., Lund Myhre et al., 2007; Stone et al., 2008; Lisok et al., 2018). For
example, a BB smoke transport event from North America to the high-Arctic
region of Svalbard in early July 2015 led to the 500 nm AOD exceeding 1.2 at
Spitsbergen (Markowicz et al., 2016). The 2 d mean aerosol direct
radiative forcing was estimated to cause overall cooling (<inline-formula><mml:math id="M3" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">79</mml:mn></mml:mrow></mml:math></inline-formula> W m<inline-formula><mml:math id="M4" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> at
the surface and <inline-formula><mml:math id="M5" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">47</mml:mn></mml:mrow></mml:math></inline-formula> W m<inline-formula><mml:math id="M6" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> at the top of the atmosphere). However, a
corresponding atmospheric heating rate profile was solved of up to 1.8 K d<inline-formula><mml:math id="M7" 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>
within the BB plume (Lisok et al., 2018). Over bright snow and ice surfaces,
or above clouds, top of the atmosphere BB smoke forcing can turn from
negative to positive (i.e., warming) by reducing columnar albedo (Yoon et
al., 2019; Markowicz et al., 2021).</p>
      <p id="d1e285">Although the microphysical impacts of aerosol particles on Arctic clouds and
precipitation processes are generally more difficult to measure and
quantify, Arctic clouds are generally believed to be more sensitive to changes in
the relatively low concentration of aerosols compared with the lower
latitudes (Prenni et al., 2007; Mauritsen et al., 2011; Birch et al., 2012;
Coopman et al., 2018; Wex et al., 2019). Extreme aerosol events correspond
with an influx of relatively large concentrations of potential cloud
condensation nuclei (CCN) and/or ice-nucleating particles (INPs), in what is
otherwise a comparatively pristine background environment (Mauritsen et al.,
2011; Leck and Svensson, 2015). Such extreme events will accordingly have
observable impacts on cloud albedo, lifetime, phase, and probability of
precipitation (e.g., Lance et al., 2011; Zhao and Garrett, 2015; Zamora et
al., 2016; Bossioli et al., 2021) and further influence the regional energy
budget. Dry deposition (and blowing snow processes), as well as wet
deposition of BB smoke particles, can also trigger sustained surface
radiative forcing by inducing surface snow discoloration and attendant
surface albedo reduction (Warren and Wiscombe, 1980; Stohl et al., 2007;
Hadley and Kirchstetter, 2012).</p>
      <p id="d1e289">Extreme aerosol events, especially BB smoke events, often modulate the
interannual variability of Arctic AOD (Xian et al.,
2022), as well as to the total annual aerosol budget in the Arctic. The
modeling study by DeRepentigny et al. (2021) shows, in comparison with BB
emissions characterized by a fixed annual cycle, that the inclusion of
interannually varying BB emissions leads to larger Arctic climate
variability and enhanced sea ice loss. Their finding illustrates the unique
sensitivity of climate-relevant processes to regional aerosol interannual
variability and further suggests that extreme aerosol events play an
important Arctic climate role. It is accordingly important to understand how
extreme aerosol-event statistics change with the changing Arctic climate to
better inform climate simulations and our baseline understanding of how the
region is poised to evolve.</p>
      <p id="d1e292">This is the second of two papers examining spring and summertime Arctic AOD
climatologies and their trends. In Part 1 (Xian et al., 2022), we report a
baseline Arctic AOD climatology from the AErosol RObotic NETwork (AERONET), the Maritime Aerosol Network (MAN), and satellite AOD data
for those two seasons and the skill of three reanalysis AOD products in
simulating those climatologies. The reanalyses and spaceborne retrievals
show consistent climatological spatial patterns and trends. Overall, AOD
exhibits a multi-year negative trend for springtime and a positive trend for
summertime during 2003–2019, due to an overall decrease in
sulfate/anthropogenic pollution and a significant summertime increase in BB
smoke. This second paper focuses on the statistics and trends of extreme
Arctic AOD events. The data and methods we employ are described in Sect. 2,
while results are provided in Sect. 3. Conclusions are presented in Sect. 4.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Data and methods</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>AERONET</title>
      <p id="d1e310">The AErosol RObotic NETwork (AERONET) is a federated ground-based sun
photometer network with over 600 active sites across the globe. AERONET's
Cimel photometers measure sun and sky radiance at several wavelengths,
ranging from the near-ultraviolet to the near-infrared. While the exact set
of bands depend on the model, all Cimel configurations include 440, 670, 870,
and 1020 nm bands. All the sites used here also included 380 and 500 nm
bands. The network has been providing high-accuracy daytime measurements of
aerosol optical properties since the 1990s (Holben et al., 1998, 2001). Cloud-screened and quality-assured Version 3 Level 2 AERONET
data (Giles et al., 2019) are used in this study.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><?xmltex \currentcnt{1}?><?xmltex \def\figurename{Figure}?><label>Figure 1</label><caption><p id="d1e315">Total, FM, and CM AOD at the 95th percentile (AOD<inline-formula><mml:math id="M8" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula>) for the
March–August time frame from the NAAPS-RA and the 10 AERONET sites based on
6-hourly data between 2003–2019.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/9949/2022/acp-22-9949-2022-f01.png"/>

        </fig>

      <p id="d1e333">Fine-mode (FM) and coarse-mode (CM) AOD at 550 nm are derived based on the
spectral deconvolution algorithm (SDA) of O'Neill et al. (2001, 2003) and averaged
over 6 h time bins. The same 10 AERONET sites employed in Part 1, were
selected (Fig. 1 of this paper) for this study. Those sites had been chosen based on their
regional representativeness as well as the availability of data records
between January 2003 and December 2019 period of study.</p>
      <p id="d1e337">Optically thin clouds, mostly cirrus, occasionally contaminate CM aerosol
retrievals in Level 2, Version 3 AERONET data (Ranjbar et al., 2022). Data
were manually inspected and retrievals screened using Moderate Resolution Imaging Spectroradiometer (MODIS) imagery at
visible wavelengths from NASA Worldview
(<uri>https://worldview.earthdata.nasa.gov/</uri>, last access: 15 May 2022) and by
comparing the 6-hourly U.S. Navy Aerosol Analysis and
Prediction System ReAnalysis version 1 (NAAPS-RA v1) with AERONET AODs. This step is likely an
incomplete one, given the likely lower sensitivity of MODIS imagers to thin
clouds (Marquis et al., 2017). As such, CM AODs that deviate by more than
the 3<inline-formula><mml:math id="M9" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> level from the background climatological mean were also removed
(as per AboEl-Fetouh et al., 2020).</p>
</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>AERONET Marine Aerosol Network AOD datasets</title>
      <p id="d1e358">The Marine Aerosol Network (MAN) is part of the broader AERONET global
network: in this case however, it is limited to AODs collected over open
water. Handheld Microtops sun photometers are deployed during research
cruises of opportunity (Smirnov et al., 2009, 2011). Data processing is
similar to that of AERONET with product nomenclature similar to AERONET.
Level 2 data acquired above 70<inline-formula><mml:math id="M10" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N in the 2003–2019 period are used
in this study. FM and CM AOD at 550 nm are derived using the SDA and
averaged over 6 h time bins.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <label>2.3</label><title>NAAPS AOD reanalysis v1</title>
      <p id="d1e378">The Navy Aerosol Analysis and Prediction System (NAAPS) AOD reanalysis
(NAAPS-RA) v1 was developed at the U.S. Naval Research Laboratory. It
provides speciated AOD and concentrations at a global scale with
1<inline-formula><mml:math id="M11" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M12" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1<inline-formula><mml:math id="M13" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> latitude–longitude and 6 h resolution for
2003–2019 (Lynch et al., 2016). NAAPS-RA is driven by the Navy Operational
Global Analysis and Prediction System (NOGAPS; Hogan and Rosmond, 1991),
with satellite precipitation applied within the tropics to mitigate model
precipitation errors (Xian et al., 2009). NAAPS-RA features the assimilation of
quality-controlled AOD retrievals from MODIS and Multi-angle
Imaging SpectroRadiometer (MISR) (Zhang and Reid, 2006;
Hyer et al., 2011; Shi et al., 2011, 2013) with the Navy Atmospheric Variational Data Assimilation System for AOD (NAVDAS-AOD, Zhang et al., 2008). A first-order approximation of
secondary organic aerosol (SOA) processes is adopted. Production of SOA from
its precursors is assumed to be instantaneous and is included with the
original anthropogenic species to form a combined anthropogenic and biogenic
fine (ABF) species. In other words, ABF is a mixture of sulfate, BC, organic
aerosols, and secondary organic aerosols from non-BB sources. Monthly
anthropogenic emissions come from a 2000–2010 average of the ECMWF MACC
inventory (e.g., Granier et al., 2011). BB smoke is derived from the Fire
Locating and Modeling of Burning Emissions inventory (FLAMBE, Reid et al.,
2009). This version of FLAMBE uses MODIS near-real-time satellite-based
thermal anomaly data to initialize the smoke source where corrections that
minimize the impact of inter-orbit variations are applied to the MODIS data
(Lynch et al., 2016). FLAMBE processing is applied consistently through the
reanalysis time period while a smoke particle emission climatology and its
spring and summertime trends (both north of 50 and
60<inline-formula><mml:math id="M14" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) are provided in Fig. 12 of Part 1 (Xian et al., 2022). Dust is emitted
dynamically and is a function of modeled friction velocity to the fourth
power, surface wetness, and surface erodibility. In this model run,
erodibility is adopted from Ginoux et al. (2001) with regional tuning.
Sea salt modeling is the same as Witek et al. (2007), and sea salt emission
is driven dynamically by sea surface wind.</p>

<?xmltex \floatpos{p}?><table-wrap id="Ch1.T1" orientation="landscape"><?xmltex \currentcnt{1}?><label>Table 1</label><caption><p id="d1e418">Geographical coordinates along with the total, FM, and CM AOD
statistics (2003–2019 depending on availability) for AERONET and 6-hourly
NAAPS-RA 550 nm performance indicators versus AERONET. These numbers are given as information: as indicated above,
the table statistics in Part 1 were explicitly computed using monthly binned
data (which were, in turn, derived from the 6 h data). The second to last  row shows
the same statistics for MAN AODs acquired north of 70<inline-formula><mml:math id="M15" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N as the
bias reference. “<inline-formula><mml:math id="M16" display="inline"><mml:mi>n</mml:mi></mml:math></inline-formula>” represents the
total number of 6 h AODs for 2003–2019, including a small amount of AERONET data from September besides the March–August time frame.</p></caption><oasis:table frame="topbot"><?xmltex \begin{scaleboxenv}{.95}[.95]?><oasis:tgroup cols="18">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="left"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="right"/>
     <oasis:colspec colnum="8" colname="col8" align="right" colsep="1"/>
     <oasis:colspec colnum="9" colname="col9" align="right"/>
     <oasis:colspec colnum="10" colname="col10" align="right"/>
     <oasis:colspec colnum="11" colname="col11" align="right" colsep="1"/>
     <oasis:colspec colnum="12" colname="col12" align="right"/>
     <oasis:colspec colnum="13" colname="col13" align="right"/>
     <oasis:colspec colnum="14" colname="col14" align="right" colsep="1"/>
     <oasis:colspec colnum="15" colname="col15" align="right"/>
     <oasis:colspec colnum="16" colname="col16" align="right"/>
     <oasis:colspec colnum="17" colname="col17" align="right" colsep="1"/>
     <oasis:colspec colnum="18" colname="col18" align="right"/>
     <oasis:thead>
       <oasis:row>
         <oasis:entry colname="col1">Sites</oasis:entry>
         <oasis:entry colname="col2">Latitude</oasis:entry>
         <oasis:entry colname="col3">Longitude</oasis:entry>
         <oasis:entry colname="col4">Elevation (m)</oasis:entry>
         <oasis:entry colname="col5">Region</oasis:entry>
         <oasis:entry rowsep="1" namest="col6" nameend="col8" align="center" colsep="1">AERONET mean </oasis:entry>
         <oasis:entry rowsep="1" namest="col9" nameend="col18" align="center">Total <inline-formula><mml:math id="M17" display="inline"><mml:mo>|</mml:mo></mml:math></inline-formula> FM <inline-formula><mml:math id="M18" display="inline"><mml:mo>|</mml:mo></mml:math></inline-formula> CM AOD </oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6">total</oasis:entry>
         <oasis:entry colname="col7">FM</oasis:entry>
         <oasis:entry colname="col8">CM</oasis:entry>
         <oasis:entry namest="col9" nameend="col11" align="center" colsep="1">Bias </oasis:entry>
         <oasis:entry namest="col12" nameend="col14" align="center" colsep="1">RMSE </oasis:entry>
         <oasis:entry namest="col15" nameend="col17" align="center" colsep="1"><inline-formula><mml:math id="M19" 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="col18"><inline-formula><mml:math id="M20" display="inline"><mml:mi>n</mml:mi></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Hornsund</oasis:entry>
         <oasis:entry colname="col2">77.0<inline-formula><mml:math id="M21" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">15.6<inline-formula><mml:math id="M22" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E</oasis:entry>
         <oasis:entry colname="col4">12</oasis:entry>
         <oasis:entry colname="col5">Svalbard</oasis:entry>
         <oasis:entry colname="col6">0.09</oasis:entry>
         <oasis:entry colname="col7">0.06</oasis:entry>
         <oasis:entry colname="col8">0.03</oasis:entry>
         <oasis:entry colname="col9"><inline-formula><mml:math id="M23" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M24" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.04</oasis:entry>
         <oasis:entry colname="col13">0.04</oasis:entry>
         <oasis:entry colname="col14">0.03</oasis:entry>
         <oasis:entry colname="col15">0.55</oasis:entry>
         <oasis:entry colname="col16">0.62</oasis:entry>
         <oasis:entry colname="col17">0.06</oasis:entry>
         <oasis:entry colname="col18">1975</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Thule</oasis:entry>
         <oasis:entry colname="col2">76.5<inline-formula><mml:math id="M25" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">68.8<inline-formula><mml:math id="M26" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W</oasis:entry>
         <oasis:entry colname="col4">225</oasis:entry>
         <oasis:entry colname="col5">Greenland</oasis:entry>
         <oasis:entry colname="col6">0.07</oasis:entry>
         <oasis:entry colname="col7">0.06</oasis:entry>
         <oasis:entry colname="col8">0.02</oasis:entry>
         <oasis:entry colname="col9">0.00</oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M27" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.04</oasis:entry>
         <oasis:entry colname="col13">0.03</oasis:entry>
         <oasis:entry colname="col14">0.03</oasis:entry>
         <oasis:entry colname="col15">0.52</oasis:entry>
         <oasis:entry colname="col16">0.60</oasis:entry>
         <oasis:entry colname="col17">0.07</oasis:entry>
         <oasis:entry colname="col18">2934</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Kangerlussuaq</oasis:entry>
         <oasis:entry colname="col2">67.0<inline-formula><mml:math id="M28" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">50.6<inline-formula><mml:math id="M29" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W</oasis:entry>
         <oasis:entry colname="col4">320</oasis:entry>
         <oasis:entry colname="col5">Greenland</oasis:entry>
         <oasis:entry colname="col6">0.07</oasis:entry>
         <oasis:entry colname="col7">0.05</oasis:entry>
         <oasis:entry colname="col8">0.02</oasis:entry>
         <oasis:entry colname="col9">0.02</oasis:entry>
         <oasis:entry colname="col10">0.00</oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.05</oasis:entry>
         <oasis:entry colname="col13">0.04</oasis:entry>
         <oasis:entry colname="col14">0.03</oasis:entry>
         <oasis:entry colname="col15">0.32</oasis:entry>
         <oasis:entry colname="col16">0.30</oasis:entry>
         <oasis:entry colname="col17">0.03</oasis:entry>
         <oasis:entry colname="col18">3066</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Ittoqqortoormiit</oasis:entry>
         <oasis:entry colname="col2">70.5<inline-formula><mml:math id="M30" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">21.0<inline-formula><mml:math id="M31" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W</oasis:entry>
         <oasis:entry colname="col4">68</oasis:entry>
         <oasis:entry colname="col5">Greenland</oasis:entry>
         <oasis:entry colname="col6">0.06</oasis:entry>
         <oasis:entry colname="col7">0.05</oasis:entry>
         <oasis:entry colname="col8">0.02</oasis:entry>
         <oasis:entry colname="col9">0.01</oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M32" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.00</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.04</oasis:entry>
         <oasis:entry colname="col13">0.03</oasis:entry>
         <oasis:entry colname="col14">0.03</oasis:entry>
         <oasis:entry colname="col15">0.41</oasis:entry>
         <oasis:entry colname="col16">0.49</oasis:entry>
         <oasis:entry colname="col17">0.04</oasis:entry>
         <oasis:entry colname="col18">2041</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Andenes</oasis:entry>
         <oasis:entry colname="col2">69.3<inline-formula><mml:math id="M33" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">16.0<inline-formula><mml:math id="M34" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E</oasis:entry>
         <oasis:entry colname="col4">379</oasis:entry>
         <oasis:entry colname="col5">Norway</oasis:entry>
         <oasis:entry colname="col6">0.08</oasis:entry>
         <oasis:entry colname="col7">0.05</oasis:entry>
         <oasis:entry colname="col8">0.02</oasis:entry>
         <oasis:entry colname="col9">0.01</oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M35" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.04</oasis:entry>
         <oasis:entry colname="col13">0.03</oasis:entry>
         <oasis:entry colname="col14">0.03</oasis:entry>
         <oasis:entry colname="col15">0.54</oasis:entry>
         <oasis:entry colname="col16">0.56</oasis:entry>
         <oasis:entry colname="col17">0.16</oasis:entry>
         <oasis:entry colname="col18">2222</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Resolute_Bay</oasis:entry>
         <oasis:entry colname="col2">74.7<inline-formula><mml:math id="M36" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">94.9<inline-formula><mml:math id="M37" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W</oasis:entry>
         <oasis:entry colname="col4">35</oasis:entry>
         <oasis:entry colname="col5">Nunavut</oasis:entry>
         <oasis:entry colname="col6">0.08</oasis:entry>
         <oasis:entry colname="col7">0.05</oasis:entry>
         <oasis:entry colname="col8">0.02</oasis:entry>
         <oasis:entry colname="col9">0.01</oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M38" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.06</oasis:entry>
         <oasis:entry colname="col13">0.05</oasis:entry>
         <oasis:entry colname="col14">0.03</oasis:entry>
         <oasis:entry colname="col15">0.55</oasis:entry>
         <oasis:entry colname="col16">0.62</oasis:entry>
         <oasis:entry colname="col17">0.02</oasis:entry>
         <oasis:entry colname="col18">1876</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Barrow</oasis:entry>
         <oasis:entry colname="col2">71.3<inline-formula><mml:math id="M39" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">156.7<inline-formula><mml:math id="M40" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W</oasis:entry>
         <oasis:entry colname="col4">8</oasis:entry>
         <oasis:entry colname="col5">Alaska</oasis:entry>
         <oasis:entry colname="col6">0.10</oasis:entry>
         <oasis:entry colname="col7">0.08</oasis:entry>
         <oasis:entry colname="col8">0.02</oasis:entry>
         <oasis:entry colname="col9"><inline-formula><mml:math id="M41" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.00</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M42" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.09</oasis:entry>
         <oasis:entry colname="col13">0.08</oasis:entry>
         <oasis:entry colname="col14">0.04</oasis:entry>
         <oasis:entry colname="col15">0.53</oasis:entry>
         <oasis:entry colname="col16">0.61</oasis:entry>
         <oasis:entry colname="col17">0.07</oasis:entry>
         <oasis:entry colname="col18">1920</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Bonanza_Creek</oasis:entry>
         <oasis:entry colname="col2">64.7<inline-formula><mml:math id="M43" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">148.3<inline-formula><mml:math id="M44" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W</oasis:entry>
         <oasis:entry colname="col4">353</oasis:entry>
         <oasis:entry colname="col5">Alaska</oasis:entry>
         <oasis:entry colname="col6">0.16</oasis:entry>
         <oasis:entry colname="col7">0.12</oasis:entry>
         <oasis:entry colname="col8">0.03</oasis:entry>
         <oasis:entry colname="col9"><inline-formula><mml:math id="M45" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M46" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11"><inline-formula><mml:math id="M47" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.00</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col12">0.16</oasis:entry>
         <oasis:entry colname="col13">0.15</oasis:entry>
         <oasis:entry colname="col14">0.04</oasis:entry>
         <oasis:entry colname="col15">0.69</oasis:entry>
         <oasis:entry colname="col16">0.70</oasis:entry>
         <oasis:entry colname="col17">0.07</oasis:entry>
         <oasis:entry colname="col18">3177</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Tiksi</oasis:entry>
         <oasis:entry colname="col2">71.6<inline-formula><mml:math id="M48" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">129.0<inline-formula><mml:math id="M49" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E</oasis:entry>
         <oasis:entry colname="col4">17</oasis:entry>
         <oasis:entry colname="col5">Siberia</oasis:entry>
         <oasis:entry colname="col6">0.12</oasis:entry>
         <oasis:entry colname="col7">0.10</oasis:entry>
         <oasis:entry colname="col8">0.02</oasis:entry>
         <oasis:entry colname="col9"><inline-formula><mml:math id="M50" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M51" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.09</oasis:entry>
         <oasis:entry colname="col13">0.08</oasis:entry>
         <oasis:entry colname="col14">0.03</oasis:entry>
         <oasis:entry colname="col15">0.69</oasis:entry>
         <oasis:entry colname="col16">0.73</oasis:entry>
         <oasis:entry colname="col17">0.01</oasis:entry>
         <oasis:entry colname="col18">631</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Yakutsk</oasis:entry>
         <oasis:entry colname="col2">61.7<inline-formula><mml:math id="M52" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">129.4<inline-formula><mml:math id="M53" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E</oasis:entry>
         <oasis:entry colname="col4">119</oasis:entry>
         <oasis:entry colname="col5">Siberia</oasis:entry>
         <oasis:entry colname="col6">0.16</oasis:entry>
         <oasis:entry colname="col7">0.12</oasis:entry>
         <oasis:entry colname="col8">0.03</oasis:entry>
         <oasis:entry colname="col9"><inline-formula><mml:math id="M54" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M55" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.13</oasis:entry>
         <oasis:entry colname="col13">0.12</oasis:entry>
         <oasis:entry colname="col14">0.04</oasis:entry>
         <oasis:entry colname="col15">0.61</oasis:entry>
         <oasis:entry colname="col16">0.62</oasis:entry>
         <oasis:entry colname="col17">0.15</oasis:entry>
         <oasis:entry colname="col18">4797</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">MAN</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M56" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">70</mml:mn></mml:mrow></mml:math></inline-formula><inline-formula><mml:math id="M57" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col3">–</oasis:entry>
         <oasis:entry colname="col4">–</oasis:entry>
         <oasis:entry colname="col5">Arctic Ocean</oasis:entry>
         <oasis:entry colname="col6">0.07</oasis:entry>
         <oasis:entry colname="col7">0.05</oasis:entry>
         <oasis:entry colname="col8">0.02</oasis:entry>
         <oasis:entry colname="col9"><inline-formula><mml:math id="M58" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.00</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M59" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.00</oasis:entry>
         <oasis:entry colname="col12">0.04</oasis:entry>
         <oasis:entry colname="col13">0.03</oasis:entry>
         <oasis:entry colname="col14">0.02</oasis:entry>
         <oasis:entry colname="col15">0.51</oasis:entry>
         <oasis:entry colname="col16">0.32</oasis:entry>
         <oasis:entry colname="col17">0.07</oasis:entry>
         <oasis:entry colname="col18">520</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">All AERONET sites</oasis:entry>
         <oasis:entry namest="col2" nameend="col5" align="center">total <inline-formula><mml:math id="M60" display="inline"><mml:mo>|</mml:mo></mml:math></inline-formula> FM <inline-formula><mml:math id="M61" display="inline"><mml:mo>|</mml:mo></mml:math></inline-formula> CM median: 0.07 <inline-formula><mml:math id="M62" display="inline"><mml:mo>|</mml:mo></mml:math></inline-formula> 0.05 <inline-formula><mml:math id="M63" display="inline"><mml:mo>|</mml:mo></mml:math></inline-formula> 0.01 </oasis:entry>
         <oasis:entry colname="col6">0.10</oasis:entry>
         <oasis:entry colname="col7">0.08</oasis:entry>
         <oasis:entry colname="col8">0.02</oasis:entry>
         <oasis:entry colname="col9"><inline-formula><mml:math id="M64" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.00</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col10"><inline-formula><mml:math id="M65" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col11">0.01</oasis:entry>
         <oasis:entry colname="col12">0.09</oasis:entry>
         <oasis:entry colname="col13">0.08</oasis:entry>
         <oasis:entry colname="col14">0.03</oasis:entry>
         <oasis:entry colname="col15">0.63</oasis:entry>
         <oasis:entry colname="col16">0.66</oasis:entry>
         <oasis:entry colname="col17">0.07</oasis:entry>
         <oasis:entry colname="col18">24 639</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup><?xmltex \end{scaleboxenv}?></oasis:table></table-wrap>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><?xmltex \currentcnt{2}?><?xmltex \def\figurename{Figure}?><label>Figure 2</label><caption><p id="d1e1667">Comparison of the 6-hourly NAAPS-RA and pairwise AERONET V3L2 data for <bold>(a)</bold> total AOD and <bold>(b)</bold> FM AOD at 550 nm. The segments from the top to the bottom of the box and whiskers represent, in order, the 95th, 90th, 75th, 50th, 25th, 10th, and 5th percentiles of data for the 10 AERONET sites of
Table 1 and Fig. 1 for the 2003–2019 time period. Also shown are the site
means of the NAAPS-RA and AERONET AODs and the NAAPS-RA RMSE, the
coefficient of determination (<inline-formula><mml:math id="M66" 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>) between the NAAPS-RA and AERONET, and
the maximum AERONET and NAAPS-RA AODs. Note that values greater than 3.0 are
not shown.</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/9949/2022/acp-22-9949-2022-f02.png"/>

        </fig>

      <p id="d1e1694">Verification of monthly binned NAAPS-RA total AODs at 550 nm using
monthly binned AERONET data from 10 Arctic sites (Tables 2–4 of Part 1, Xian et al., 2022) shows that NAAPS-RA is able to capture the AOD interannual variability.
The spatial distributions and magnitudes of climatological and seasonal AOD
averages and their trends for 2003–2019 are also consistent with those
derived from MODIS, MISR, and the Cloud-Aerosol Lidar with Orthogonal
Polarization (CALIOP) (Part 1). NAAPS-RA is also shown to be able to capture biomass burning smoke transport events into the polar regions in various case studies (e.g., Markowicz et al., 2016, 2017; Khan et al., 2017, 2018, 2019; Ranjbar et al., 2019; AboEl-Fetouh et al., 2022).</p>
</sec>
<sec id="Ch1.S2.SS4">
  <label>2.4</label><title>Data analysis methods</title>
      <p id="d1e1705">Our study period is January 2003 to December 2019, the same principal study period as
used in Part 1. We define extreme events as those corresponding to AOD
exceeding the 95th percentile mark in 6 h or daily AOD data at a
specific location or across a given region (the region north of
70<inline-formula><mml:math id="M67" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N for example). We employ 6 h AERONET AODs as well as
speciated daily and 6 h NAAPS-RA AOD to depict the frequency and magnitude
of the large FM AOD events. Pairwise data are used for verification.
“Pairwise” refers to those NAAPS-RA AODs that correspond to a resampled
AERONET or MAN AOD whose <inline-formula><mml:math id="M68" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula> h bin contains at least one AERONET/MAN
retrieval. Three independent aerosol reanalysis products were used in Part 1 of the study. For this study, the NAAPS-RA reanalysis was chosen
given its slightly better performance in terms of FM and total-AOD bias,
RMSE, and <inline-formula><mml:math id="M69" 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> scores (Part 1) as well as its capability of separating
BB smoke from other aerosol species. To simplify some of the discussion
below, we frequently employed the symbol “AOD<inline-formula><mml:math id="M70" display="inline"><mml:msub><mml:mi/><mml:mi>n</mml:mi></mml:msub></mml:math></inline-formula>” to represent the AOD
associated with the <inline-formula><mml:math id="M71" display="inline"><mml:mi>n</mml:mi></mml:math></inline-formula>th percentile of its cumulative (histogram)
distribution. One important application of this AOD<inline-formula><mml:math id="M72" display="inline"><mml:msub><mml:mi/><mml:mi>n</mml:mi></mml:msub></mml:math></inline-formula> formulation is to
employ a particular value (AOD<inline-formula><mml:math id="M73" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula>) as a threshold for the definition of
extreme events (see Sect. 3.1 below). AOD<inline-formula><mml:math id="M74" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">75</mml:mn></mml:msub></mml:math></inline-formula>, AOD<inline-formula><mml:math id="M75" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">90</mml:mn></mml:msub></mml:math></inline-formula>, AOD<inline-formula><mml:math id="M76" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">99</mml:mn></mml:msub></mml:math></inline-formula>,
AOD<inline-formula><mml:math id="M77" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">99.5</mml:mn></mml:msub></mml:math></inline-formula>, and maximum AOD are also calculated to show AOD gradients for
high AODs. A local extreme total-AOD event for the NAAPS-RA means AOD
&gt;AOD<inline-formula><mml:math id="M78" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> for the model grid cell of 1<inline-formula><mml:math id="M79" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M80" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1<inline-formula><mml:math id="M81" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> (latitude–longitude). Again, we define the Arctic and the
high Arctic as regions north of 60 and 70<inline-formula><mml:math id="M82" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N,
respectively. To reference source influences from lower latitudes, the area
of 50–90<inline-formula><mml:math id="M83" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N is included for context.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Results</title>
      <p id="d1e1871">Regional statistics and trends of extreme AOD events are presented in this
section: 6 h AERONET AOD as well as speciated daily and 6 h NAAPS-RA AOD
are employed to characterize the frequency and magnitude of strong FM AOD
events.</p>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Verification of NAAPS-RA AOD over the Arctic</title>
      <p id="d1e1881">The reanalysis performance for 6 h time bins was evaluated in order to
study extreme events. Our choice of AOD<inline-formula><mml:math id="M84" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> as an extreme-event threshold
was influenced by the fact that it was an upper-limit cumulative probability
indicator that was robust. We reasoned, at the same time, that it should be
comparable with the analog parameter derived from NAAPS-RA. Figure 1
displays NAAPS-RA AOD<inline-formula><mml:math id="M85" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> overplotted with those from the 10 selected
AERONET sites for spring and summertime 2003–2019. NAAPS-RA appears to
successfully capture the AOD<inline-formula><mml:math id="M86" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> amplitude and spatial pattern as well
as those of FM AOD<inline-formula><mml:math id="M87" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> and CM AOD<inline-formula><mml:math id="M88" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula>. It also shows that FM is the
main contributor to AOD<inline-formula><mml:math id="M89" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> in the Arctic.</p>
      <p id="d1e1939">Detailed geographical coordinates of the 10 AERONET sites employed in our
study are included in Table 1 as well as the simulation performance
indicators of NAAPS-RA 550 nm total, FM, and CM AOD. These AERONET parameters
are an analog to parameters used in the first part of the study and its
Table 1 statistics, except that the averaging period extends across both the
spring and summer seasons, as the averaging period is mostly confined to the
April–August time frame. NAAPS-RA performance indicators relative to MAN
data are shown in Figs. S1 and S2.</p>
      <p id="d1e1942">NAAPS-RA performance for this large averaging period is reasonable for FM
and total AOD, though it is less skillful at predicting CM AOD. The FM AOD
exhibits an average (Table 1) bias over all stations of <inline-formula><mml:math id="M90" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula>, a root-mean-square error (RMSE) of 0.08, and a coefficient of determination
(<inline-formula><mml:math id="M91" 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>) of 0.66. RMSE values for total and FM AOD are generally
large for sites vulnerable to strong smoke influence, e.g., Bonanza Creek,
Barrow, Tiksi, and Yakutsk. Total-AOD <inline-formula><mml:math id="M92" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> values are mostly between
0.5–0.7 except for Kangerlussuaq and Ittoqqortoormiit. FM AOD
<inline-formula><mml:math id="M93" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> values exceed those of the total AOD for all sites except
Kangerlussuaq. The 6 h binned Table 1 total-AOD bias is similar to the
monthly binned NAAPS-RA bias results of Table 2 in Part 1 (Xian et al., 2022). This is due to the
numerous 6 h samples included in the averaging process. In contrast,
the Table 1 RMSE values are roughly doubled, and the <inline-formula><mml:math id="M94" display="inline"><mml:mrow><mml:msup><mml:mi>r</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> values drop by
about 20 % relative to those of Tables 3 and 4 of Part 1 (Xian et al., 2022). This suggests
Table 1 model shortcomings in capturing finer temporal-scale AERONET-AOD
variations. This is also consistent with model performance for regions other
than the Arctic and is generally a common result for numerical aerosol
models (Lynch et al., 2016; Yumimoto et al., 2017)</p>
      <p id="d1e1999">The lower CM vs. FM skill of the NAAPS-RA might be a reflection of AERONET
limitations as one approaches typical instrumental errors <inline-formula><mml:math id="M95" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula> in total AOD or they could be a reflection of simulation and/or
reanalysis limitations as one approaches very small values of CM AOD. The
lack of model representation of CM smoke and possible soil particles
associated with severe burning events may also contribute. At the same time,
it must be recognized that residual cloud contamination in AERONET and MAN
data cannot be ruled out as a “false” indicator of poor simulation skill.
Cloud screening issues aside, a lower CM vs. FM correlation skill is a
common feature of both the Table 1 and 4 (Part 1, Xian et al., 2022) reanalyses. However,
modeled monthly CM AOD correlation is slightly more skillful than the
averages derived from 6 h data (Table 4 in Part 1, Xian et al., 2022, vs. Table 1 in this paper) inasmuch as
the seasonal CM signal associated with dust and sea salt aerosols is apparently better resolved in the former case. The better model skill in
seasonal CM simulation is likely due to the relative insensitivity of the
model to the higher-frequency components of the reference data in the latter
case. It is also noted that the NAAPS-RA is generally less skillful in the
Arctic region relative to global reanalyses (see Fig. 7 in Lynch et al.,
2016). This is understandable given that there are little satellite-based AOD
data available to constrain the model through assimilation in the Arctic
compared to lower latitudes. We note however that Zhang et al. (2021)
attempted to address this problem with the assimilation of the Ozone Monitoring
Instrument (OMI) aerosol index. To date, no remedy for aerosol data
assimilation has yet been implemented in a larger reanalysis quality study.</p>

<?xmltex \floatpos{p}?><table-wrap id="Ch1.T2" orientation="landscape"><?xmltex \currentcnt{2}?><label>Table 2</label><caption><p id="d1e2016">AERONET V2L3 FM, CM, and total AOD at 550 nm at different
percentiles for the listed Arctic sites along with maximum AOD values in the three columns next to the last column. The percentage of extreme FM events relative to the
number of extreme total-AOD events (using our AOD<inline-formula><mml:math id="M96" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> extreme-event
threshold) is also shown in the last column. The second to last row shows
MAN statistics for data acquired north of 70<inline-formula><mml:math id="M97" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N.</p></caption><oasis:table frame="topbot"><?xmltex \begin{scaleboxenv}{.81}[.81]?><oasis:tgroup cols="24">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right" colsep="1"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="right" colsep="1"/>
     <oasis:colspec colnum="8" colname="col8" align="right"/>
     <oasis:colspec colnum="9" colname="col9" align="right"/>
     <oasis:colspec colnum="10" colname="col10" align="right" colsep="1"/>
     <oasis:colspec colnum="11" colname="col11" align="right"/>
     <oasis:colspec colnum="12" colname="col12" align="right"/>
     <oasis:colspec colnum="13" colname="col13" align="right" colsep="1"/>
     <oasis:colspec colnum="14" colname="col14" align="right"/>
     <oasis:colspec colnum="15" colname="col15" align="right"/>
     <oasis:colspec colnum="16" colname="col16" align="right" colsep="1"/>
     <oasis:colspec colnum="17" colname="col17" align="right"/>
     <oasis:colspec colnum="18" colname="col18" align="right"/>
     <oasis:colspec colnum="19" colname="col19" align="right" colsep="1"/>
     <oasis:colspec colnum="20" colname="col20" align="right"/>
     <oasis:colspec colnum="21" colname="col21" align="right"/>
     <oasis:colspec colnum="22" colname="col22" align="right"/>
     <oasis:colspec colnum="23" colname="col23" align="right"/>
     <oasis:colspec colnum="24" colname="col24" align="left"/>
     <oasis:thead>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry rowsep="1" namest="col2" nameend="col22" align="center">Total <inline-formula><mml:math id="M98" display="inline"><mml:mo>|</mml:mo></mml:math></inline-formula> FM <inline-formula><mml:math id="M99" display="inline"><mml:mo>|</mml:mo></mml:math></inline-formula> CM AOD at 550 nm </oasis:entry>
         <oasis:entry colname="col23">FM event</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry namest="col2" nameend="col4" align="center" colsep="1">Median </oasis:entry>
         <oasis:entry namest="col5" nameend="col7" align="center" colsep="1">75 % </oasis:entry>
         <oasis:entry namest="col8" nameend="col10" align="center" colsep="1">90 % </oasis:entry>
         <oasis:entry namest="col11" nameend="col13" align="center" colsep="1">95 % </oasis:entry>
         <oasis:entry namest="col14" nameend="col16" align="center" colsep="1">99 % </oasis:entry>
         <oasis:entry namest="col17" nameend="col19" align="center" colsep="1">99.9 % </oasis:entry>
         <oasis:entry namest="col20" nameend="col22" align="center">Maximum </oasis:entry>
         <oasis:entry colname="col23"/>
         <oasis:entry colname="col24"/>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Hornsund</oasis:entry>
         <oasis:entry colname="col2">0.072</oasis:entry>
         <oasis:entry colname="col3">0.049</oasis:entry>
         <oasis:entry colname="col4">0.014</oasis:entry>
         <oasis:entry colname="col5">0.103</oasis:entry>
         <oasis:entry colname="col6">0.074</oasis:entry>
         <oasis:entry colname="col7">0.028</oasis:entry>
         <oasis:entry colname="col8">0.145</oasis:entry>
         <oasis:entry colname="col9">0.108</oasis:entry>
         <oasis:entry colname="col10">0.048</oasis:entry>
         <oasis:entry colname="col11">0.184</oasis:entry>
         <oasis:entry colname="col12">0.135</oasis:entry>
         <oasis:entry colname="col13">0.077</oasis:entry>
         <oasis:entry colname="col14">0.320</oasis:entry>
         <oasis:entry colname="col15">0.300</oasis:entry>
         <oasis:entry colname="col16">0.155</oasis:entry>
         <oasis:entry colname="col17">0.663</oasis:entry>
         <oasis:entry colname="col18">0.654</oasis:entry>
         <oasis:entry colname="col19">0.222</oasis:entry>
         <oasis:entry colname="col20">0.663</oasis:entry>
         <oasis:entry colname="col21">0.654</oasis:entry>
         <oasis:entry colname="col22">0.222</oasis:entry>
         <oasis:entry colname="col23">67 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Thule</oasis:entry>
         <oasis:entry colname="col2">0.055</oasis:entry>
         <oasis:entry colname="col3">0.043</oasis:entry>
         <oasis:entry colname="col4">0.006</oasis:entry>
         <oasis:entry colname="col5">0.083</oasis:entry>
         <oasis:entry colname="col6">0.067</oasis:entry>
         <oasis:entry colname="col7">0.014</oasis:entry>
         <oasis:entry colname="col8">0.121</oasis:entry>
         <oasis:entry colname="col9">0.092</oasis:entry>
         <oasis:entry colname="col10">0.034</oasis:entry>
         <oasis:entry colname="col11">0.156</oasis:entry>
         <oasis:entry colname="col12">0.116</oasis:entry>
         <oasis:entry colname="col13">0.057</oasis:entry>
         <oasis:entry colname="col14">0.294</oasis:entry>
         <oasis:entry colname="col15">0.198</oasis:entry>
         <oasis:entry colname="col16">0.164</oasis:entry>
         <oasis:entry colname="col17">0.914</oasis:entry>
         <oasis:entry colname="col18">0.913</oasis:entry>
         <oasis:entry colname="col19">0.315</oasis:entry>
         <oasis:entry colname="col20">1.310</oasis:entry>
         <oasis:entry colname="col21">1.272</oasis:entry>
         <oasis:entry colname="col22">0.315</oasis:entry>
         <oasis:entry colname="col23">59 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Kangerlussuaq</oasis:entry>
         <oasis:entry colname="col2">0.055</oasis:entry>
         <oasis:entry colname="col3">0.040</oasis:entry>
         <oasis:entry colname="col4">0.009</oasis:entry>
         <oasis:entry colname="col5">0.082</oasis:entry>
         <oasis:entry colname="col6">0.063</oasis:entry>
         <oasis:entry colname="col7">0.020</oasis:entry>
         <oasis:entry colname="col8">0.118</oasis:entry>
         <oasis:entry colname="col9">0.091</oasis:entry>
         <oasis:entry colname="col10">0.037</oasis:entry>
         <oasis:entry colname="col11">0.149</oasis:entry>
         <oasis:entry colname="col12">0.115</oasis:entry>
         <oasis:entry colname="col13">0.059</oasis:entry>
         <oasis:entry colname="col14">0.234</oasis:entry>
         <oasis:entry colname="col15">0.198</oasis:entry>
         <oasis:entry colname="col16">0.109</oasis:entry>
         <oasis:entry colname="col17">0.510</oasis:entry>
         <oasis:entry colname="col18">0.461</oasis:entry>
         <oasis:entry colname="col19">0.203</oasis:entry>
         <oasis:entry colname="col20">0.794</oasis:entry>
         <oasis:entry colname="col21">0.786</oasis:entry>
         <oasis:entry colname="col22">0.222</oasis:entry>
         <oasis:entry colname="col23">75 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Ittoqqortoormiit</oasis:entry>
         <oasis:entry colname="col2">0.046</oasis:entry>
         <oasis:entry colname="col3">0.033</oasis:entry>
         <oasis:entry colname="col4">0.006</oasis:entry>
         <oasis:entry colname="col5">0.069</oasis:entry>
         <oasis:entry colname="col6">0.053</oasis:entry>
         <oasis:entry colname="col7">0.014</oasis:entry>
         <oasis:entry colname="col8">0.108</oasis:entry>
         <oasis:entry colname="col9">0.083</oasis:entry>
         <oasis:entry colname="col10">0.031</oasis:entry>
         <oasis:entry colname="col11">0.144</oasis:entry>
         <oasis:entry colname="col12">0.112</oasis:entry>
         <oasis:entry colname="col13">0.054</oasis:entry>
         <oasis:entry colname="col14">0.238</oasis:entry>
         <oasis:entry colname="col15">0.215</oasis:entry>
         <oasis:entry colname="col16">0.121</oasis:entry>
         <oasis:entry colname="col17">0.456</oasis:entry>
         <oasis:entry colname="col18">0.446</oasis:entry>
         <oasis:entry colname="col19">0.232</oasis:entry>
         <oasis:entry colname="col20">0.459</oasis:entry>
         <oasis:entry colname="col21">0.450</oasis:entry>
         <oasis:entry colname="col22">0.233</oasis:entry>
         <oasis:entry colname="col23">73 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Andenes</oasis:entry>
         <oasis:entry colname="col2">0.062</oasis:entry>
         <oasis:entry colname="col3">0.042</oasis:entry>
         <oasis:entry colname="col4">0.014</oasis:entry>
         <oasis:entry colname="col5">0.096</oasis:entry>
         <oasis:entry colname="col6">0.064</oasis:entry>
         <oasis:entry colname="col7">0.027</oasis:entry>
         <oasis:entry colname="col8">0.136</oasis:entry>
         <oasis:entry colname="col9">0.098</oasis:entry>
         <oasis:entry colname="col10">0.049</oasis:entry>
         <oasis:entry colname="col11">0.172</oasis:entry>
         <oasis:entry colname="col12">0.123</oasis:entry>
         <oasis:entry colname="col13">0.072</oasis:entry>
         <oasis:entry colname="col14">0.274</oasis:entry>
         <oasis:entry colname="col15">0.210</oasis:entry>
         <oasis:entry colname="col16">0.148</oasis:entry>
         <oasis:entry colname="col17">0.451</oasis:entry>
         <oasis:entry colname="col18">0.432</oasis:entry>
         <oasis:entry colname="col19">0.249</oasis:entry>
         <oasis:entry colname="col20">0.541</oasis:entry>
         <oasis:entry colname="col21">0.534</oasis:entry>
         <oasis:entry colname="col22">0.258</oasis:entry>
         <oasis:entry colname="col23">69 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Resolute_Bay</oasis:entry>
         <oasis:entry colname="col2">0.061</oasis:entry>
         <oasis:entry colname="col3">0.045</oasis:entry>
         <oasis:entry colname="col4">0.011</oasis:entry>
         <oasis:entry colname="col5">0.092</oasis:entry>
         <oasis:entry colname="col6">0.069</oasis:entry>
         <oasis:entry colname="col7">0.021</oasis:entry>
         <oasis:entry colname="col8">0.143</oasis:entry>
         <oasis:entry colname="col9">0.106</oasis:entry>
         <oasis:entry colname="col10">0.039</oasis:entry>
         <oasis:entry colname="col11">0.187</oasis:entry>
         <oasis:entry colname="col12">0.140</oasis:entry>
         <oasis:entry colname="col13">0.059</oasis:entry>
         <oasis:entry colname="col14">0.409</oasis:entry>
         <oasis:entry colname="col15">0.389</oasis:entry>
         <oasis:entry colname="col16">0.152</oasis:entry>
         <oasis:entry colname="col17">1.530</oasis:entry>
         <oasis:entry colname="col18">1.516</oasis:entry>
         <oasis:entry colname="col19">0.379</oasis:entry>
         <oasis:entry colname="col20">1.530</oasis:entry>
         <oasis:entry colname="col21">1.516</oasis:entry>
         <oasis:entry colname="col22">0.379</oasis:entry>
         <oasis:entry colname="col23">72 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Barrow</oasis:entry>
         <oasis:entry colname="col2">0.071</oasis:entry>
         <oasis:entry colname="col3">0.053</oasis:entry>
         <oasis:entry colname="col4">0.013</oasis:entry>
         <oasis:entry colname="col5">0.114</oasis:entry>
         <oasis:entry colname="col6">0.082</oasis:entry>
         <oasis:entry colname="col7">0.024</oasis:entry>
         <oasis:entry colname="col8">0.175</oasis:entry>
         <oasis:entry colname="col9">0.134</oasis:entry>
         <oasis:entry colname="col10">0.047</oasis:entry>
         <oasis:entry colname="col11">0.232</oasis:entry>
         <oasis:entry colname="col12">0.183</oasis:entry>
         <oasis:entry colname="col13">0.076</oasis:entry>
         <oasis:entry colname="col14">0.455</oasis:entry>
         <oasis:entry colname="col15">0.415</oasis:entry>
         <oasis:entry colname="col16">0.174</oasis:entry>
         <oasis:entry colname="col17">2.999</oasis:entry>
         <oasis:entry colname="col18">2.962</oasis:entry>
         <oasis:entry colname="col19">0.328</oasis:entry>
         <oasis:entry colname="col20">2.999</oasis:entry>
         <oasis:entry colname="col21">2.962</oasis:entry>
         <oasis:entry colname="col22">0.328</oasis:entry>
         <oasis:entry colname="col23">81 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Bonanza_Creek</oasis:entry>
         <oasis:entry colname="col2">0.078</oasis:entry>
         <oasis:entry colname="col3">0.048</oasis:entry>
         <oasis:entry colname="col4">0.022</oasis:entry>
         <oasis:entry colname="col5">0.130</oasis:entry>
         <oasis:entry colname="col6">0.089</oasis:entry>
         <oasis:entry colname="col7">0.036</oasis:entry>
         <oasis:entry colname="col8">0.280</oasis:entry>
         <oasis:entry colname="col9">0.230</oasis:entry>
         <oasis:entry colname="col10">0.057</oasis:entry>
         <oasis:entry colname="col11">0.532</oasis:entry>
         <oasis:entry colname="col12">0.497</oasis:entry>
         <oasis:entry colname="col13">0.083</oasis:entry>
         <oasis:entry colname="col14">1.713</oasis:entry>
         <oasis:entry colname="col15">1.643</oasis:entry>
         <oasis:entry colname="col16">0.186</oasis:entry>
         <oasis:entry colname="col17">2.619</oasis:entry>
         <oasis:entry colname="col18">2.591</oasis:entry>
         <oasis:entry colname="col19">0.341</oasis:entry>
         <oasis:entry colname="col20">2.908</oasis:entry>
         <oasis:entry colname="col21">2.857</oasis:entry>
         <oasis:entry colname="col22">0.345</oasis:entry>
         <oasis:entry colname="col23">99 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Tiksi</oasis:entry>
         <oasis:entry colname="col2">0.079</oasis:entry>
         <oasis:entry colname="col3">0.061</oasis:entry>
         <oasis:entry colname="col4">0.011</oasis:entry>
         <oasis:entry colname="col5">0.121</oasis:entry>
         <oasis:entry colname="col6">0.096</oasis:entry>
         <oasis:entry colname="col7">0.021</oasis:entry>
         <oasis:entry colname="col8">0.182</oasis:entry>
         <oasis:entry colname="col9">0.163</oasis:entry>
         <oasis:entry colname="col10">0.040</oasis:entry>
         <oasis:entry colname="col11">0.286</oasis:entry>
         <oasis:entry colname="col12">0.239</oasis:entry>
         <oasis:entry colname="col13">0.060</oasis:entry>
         <oasis:entry colname="col14">0.936</oasis:entry>
         <oasis:entry colname="col15">0.915</oasis:entry>
         <oasis:entry colname="col16">0.123</oasis:entry>
         <oasis:entry colname="col17">1.442</oasis:entry>
         <oasis:entry colname="col18">1.413</oasis:entry>
         <oasis:entry colname="col19">0.238</oasis:entry>
         <oasis:entry colname="col20">1.442</oasis:entry>
         <oasis:entry colname="col21">1.413</oasis:entry>
         <oasis:entry colname="col22">0.238</oasis:entry>
         <oasis:entry colname="col23">97 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Yakutsk</oasis:entry>
         <oasis:entry colname="col2">0.094</oasis:entry>
         <oasis:entry colname="col3">0.069</oasis:entry>
         <oasis:entry colname="col4">0.014</oasis:entry>
         <oasis:entry colname="col5">0.153</oasis:entry>
         <oasis:entry colname="col6">0.119</oasis:entry>
         <oasis:entry colname="col7">0.027</oasis:entry>
         <oasis:entry colname="col8">0.272</oasis:entry>
         <oasis:entry colname="col9">0.221</oasis:entry>
         <oasis:entry colname="col10">0.053</oasis:entry>
         <oasis:entry colname="col11">0.400</oasis:entry>
         <oasis:entry colname="col12">0.345</oasis:entry>
         <oasis:entry colname="col13">0.089</oasis:entry>
         <oasis:entry colname="col14">0.980</oasis:entry>
         <oasis:entry colname="col15">0.963</oasis:entry>
         <oasis:entry colname="col16">0.201</oasis:entry>
         <oasis:entry colname="col17">3.018</oasis:entry>
         <oasis:entry colname="col18">2.972</oasis:entry>
         <oasis:entry colname="col19">0.317</oasis:entry>
         <oasis:entry colname="col20">3.296</oasis:entry>
         <oasis:entry colname="col21">3.259</oasis:entry>
         <oasis:entry colname="col22">0.340</oasis:entry>
         <oasis:entry colname="col23">96 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">MAN</oasis:entry>
         <oasis:entry colname="col2">0.052</oasis:entry>
         <oasis:entry colname="col3">0.029</oasis:entry>
         <oasis:entry colname="col4">0.021</oasis:entry>
         <oasis:entry colname="col5">0.090</oasis:entry>
         <oasis:entry colname="col6">0.062</oasis:entry>
         <oasis:entry colname="col7">0.031</oasis:entry>
         <oasis:entry colname="col8">0.126</oasis:entry>
         <oasis:entry colname="col9">0.097</oasis:entry>
         <oasis:entry colname="col10">0.042</oasis:entry>
         <oasis:entry colname="col11">0.164</oasis:entry>
         <oasis:entry colname="col12">0.118</oasis:entry>
         <oasis:entry colname="col13">0.052</oasis:entry>
         <oasis:entry colname="col14">0.281</oasis:entry>
         <oasis:entry colname="col15">0.253</oasis:entry>
         <oasis:entry colname="col16">0.085</oasis:entry>
         <oasis:entry colname="col17">0.777</oasis:entry>
         <oasis:entry colname="col18">0.761</oasis:entry>
         <oasis:entry colname="col19">0.234</oasis:entry>
         <oasis:entry colname="col20">0.777</oasis:entry>
         <oasis:entry colname="col21">0.761</oasis:entry>
         <oasis:entry colname="col22">0.234</oasis:entry>
         <oasis:entry colname="col23">92 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">All AERONET sites</oasis:entry>
         <oasis:entry colname="col2">0.066</oasis:entry>
         <oasis:entry colname="col3">0.047</oasis:entry>
         <oasis:entry colname="col4">0.012</oasis:entry>
         <oasis:entry colname="col5">0.104</oasis:entry>
         <oasis:entry colname="col6">0.077</oasis:entry>
         <oasis:entry colname="col7">0.024</oasis:entry>
         <oasis:entry colname="col8">0.166</oasis:entry>
         <oasis:entry colname="col9">0.128</oasis:entry>
         <oasis:entry colname="col10">0.046</oasis:entry>
         <oasis:entry colname="col11">0.243</oasis:entry>
         <oasis:entry colname="col12">0.193</oasis:entry>
         <oasis:entry colname="col13">0.070</oasis:entry>
         <oasis:entry colname="col14">0.661</oasis:entry>
         <oasis:entry colname="col15">0.619</oasis:entry>
         <oasis:entry colname="col16">0.158</oasis:entry>
         <oasis:entry colname="col17">2.073</oasis:entry>
         <oasis:entry colname="col18">2.030</oasis:entry>
         <oasis:entry colname="col19">0.290</oasis:entry>
         <oasis:entry colname="col20">3.296</oasis:entry>
         <oasis:entry colname="col21">3.259</oasis:entry>
         <oasis:entry colname="col22">0.379</oasis:entry>
         <oasis:entry colname="col23">86 %</oasis:entry>
         <oasis:entry colname="col24"/>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup><?xmltex \end{scaleboxenv}?></oasis:table></table-wrap>

</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><title>General statistics of extreme events</title>
      <p id="d1e3104">Shown in Fig. 1 are NAAPS-RA and AERONET AOD<inline-formula><mml:math id="M100" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> values for
the March–August time frame and the 2003–2019 period. The values of
AOD<inline-formula><mml:math id="M101" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> are high (0.4–0.55) over Siberia and Alaska (and
over the Yakutsk and Bonanza Creek AERONET stations) due to strong BB smoke
influence. North of 70<inline-formula><mml:math id="M102" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, the values are mostly between 0.15 to
0.25, with the exception of Greenland where they are largely below 0.15
(weak values that are attributable to the high terrain). It is also shown
that (FM AOD)<inline-formula><mml:math id="M103" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> has a similar spatial distribution and magnitude as
AOD<inline-formula><mml:math id="M104" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula>, suggesting the dominant contribution of FM to AOD<inline-formula><mml:math id="M105" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula>. The contribution of CM is relatively larger over the North Atlantic and
European Arctic, though (CM AOD)<inline-formula><mml:math id="M106" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> and (FM AOD)<inline-formula><mml:math id="M107" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> are
comparable in these regions.</p>
      <p id="d1e3180">The site-by-site, total, and FM AOD ranges are also shown in Fig. 2 from the
6 h AERONET data for all 550 nm retrievals acquired between 2003–2019. In
general, the NAAPS-RA largely captures the AERONET FM and total-AOD range.
This includes, for example, the AERONET AOD<inline-formula><mml:math id="M108" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">5</mml:mn></mml:msub></mml:math></inline-formula> to AOD<inline-formula><mml:math id="M109" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> values
(0.02 to <inline-formula><mml:math id="M110" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">0.10</mml:mn></mml:mrow></mml:math></inline-formula> for most sites), and the larger 0.02 to 0.4–0.6
range of sites with a known strong BB influence (notably Bonanza Creek
and Yakutsk). Mean and median AODs are also comparable to AERONET values.
Maximum AERONET FM AODs vary between 0.5 (Ittoqqortoormiit) to <inline-formula><mml:math id="M111" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">2.0</mml:mn></mml:mrow></mml:math></inline-formula>
for most sites and around 3.0 for sites with strong BB smoke influence (see
also Table 2). Maximum NAAPS-RA AOD values are often biased low, which is a
common challenge for global aerosol models (e.g., Sessions et al., 2015; Xian
et al., 2019).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e3223"><bold>(a, b)</bold> Cumulative probability distributions of
2003–2019, 6 h total, FM, and CM AOD at 550 nm for AERONET V3 L2 data (solid
curves) and pairwise NAAPS-RA (dashed curves). <bold>(c, d)</bold> Cumulative probability distributions for the corresponding speciated AOD
from the NAAPS-RA. <bold>(a, c)</bold> AOD for sites that are distant
from BB source regions, including Barrow, Resolute Bay, Kangerlussuaq,
Thule, Andenes, Hornsund and Ittoqqortoormiit (see the discussion of Fig. 3
for emission considerations with respect to the particular site of Barrow).
<bold>(b)</bold>, <bold>(d)</bold> All sites. “<inline-formula><mml:math id="M112" display="inline"><mml:mi>n</mml:mi></mml:math></inline-formula>” represents the total number of
6-hourly data points over the 2003–2019 period.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/9949/2022/acp-22-9949-2022-f03.png"/>

        </fig>

      <p id="d1e3254">The cumulative probability distributions of 6 h total, FM, and CM AODs are
shown in Fig. 3 for AERONET and pairwise NAAPS-RA total and modal AODs and
speciated AODs. The median AOD for all AERONET sites in the Arctic (all
sites north of 60<inline-formula><mml:math id="M113" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) for 2003–2019 is 0.07, while the AOD<inline-formula><mml:math id="M114" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula>
extreme-event threshold is 0.24 with a dominant FM contribution (see also Table 2). The CM AOD
median for all measurements is 0.01, with a (CM AOD)<inline-formula><mml:math id="M115" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> threshold of
only 0.07. Due to a relatively large positive bias in CM AOD of 0.01 below the 95 % threshold, NAAPS-RA total-AOD bias is slightly positive
(<inline-formula><mml:math id="M116" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula>) for all sites north of 60<inline-formula><mml:math id="M117" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and for the
20 %–80 % cumulative probability range (a positive bias that is
generally evident in Table 1).</p>
      <p id="d1e3303">The negative bias found at the largest CM AOD values could conceivably be
associated with an underestimation of the CM AOD generated by sea salt
aerosols or local dust in the presence of strong winds or CM smoke and soil particles
associated with severe burnings. We should, however, reemphasize this
caveat: despite the quality control measures taken to filter out
cloud-contaminated AERONET data, the impact of CM residual clouds may still
influence estimates of CM AOD.</p>
      <p id="d1e3306">It is worth noting that BB smoke plays a dominant role compared to other
aerosol species above our AOD<inline-formula><mml:math id="M118" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> extreme-event threshold (see Fig. 3c and d
in particular and note that Fig. 3a and b show the expected dominance of FM
AOD). Even for sites distant from BB source regions, including Resolute Bay,
Kangerlussuaq, Thule, Andenes, Hornsund, and Ittoqqortoormiit, BB smoke is the
principal driver of AOD variations above the AOD<inline-formula><mml:math id="M119" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> threshold. To some
extent, Barrow can be categorized as being a site that is distant from BB
emissions. However, it is also relatively close to the region of Alaska
fires, depending on dominant upstream winds and trajectories (see Eck et
al., 2009, for details).</p>
      <p id="d1e3327">The modal and total-AOD values at different percentile levels for the
AERONET sites and MAN data collected north of 70<inline-formula><mml:math id="M120" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N are provided
in Table 2. For sites closer to BB sources, including Bonanza Creek,
Yakutsk, and Tiksi, the AOD<inline-formula><mml:math id="M121" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">99</mml:mn></mml:msub></mml:math></inline-formula> and (FM AOD)<inline-formula><mml:math id="M122" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">99</mml:mn></mml:msub></mml:math></inline-formula> values are around or larger
than 1.0, while the maximum values are between 1.4–3.3. For the more distant
sites, the AOD<inline-formula><mml:math id="M123" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">99</mml:mn></mml:msub></mml:math></inline-formula> and (FM AOD)<inline-formula><mml:math id="M124" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">99</mml:mn></mml:msub></mml:math></inline-formula> values vary between 0.23–0.46, while the maximum values are between 0.45–3.0 (1.5 for Resolute Bay and 3.0
for Barrow). The FM event occurrences for the extreme total-AOD events range
from 60 %–99 %, with an average of 86 %, and accordingly dominate CM
events statistically. Sites closer to the BB source regions show relative
occurrences over 95 %.</p>
      <p id="d1e3375">Large particles like ash and soil components emitted from vigorous burning
during extreme BB smoke events (Reid et al., 2005; Schlosser et al., 2017)
can likely be detected as AERONET CM AOD (see, for example, the correlation
between the FM and “weak” CM particle size distributions for Bonanza Creek
in Fig. 9a of Eck et al., 2009). The extreme AOD events described above are
likely dominated by smoke. For example, (FM AOD)<inline-formula><mml:math id="M125" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">99</mml:mn></mml:msub></mml:math></inline-formula> is 1.64 at Bonanza
Creek and 0.92 at Tiksi in Table 2. For events with FM AOD greater than (FM
AOD)<inline-formula><mml:math id="M126" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">99</mml:mn></mml:msub></mml:math></inline-formula>, the associated CM AOD means at the two sites showed
significantly larger values of 0.05 and 0.03 (significantly
larger relative to, for example, the CM AOD means in Table 1). The coherency
of the associated CM AOD mean increase with the FM AOD mean increase
suggests the presence of detectable CM smoke and/or soil particles induced
by severe burning. The inability of the model to simulate potential CM smoke
or soil components associated with severe burning could be a contributing
reason as to why it performs less well in predicting CM AOD near BB sites.</p>
</sec>
<sec id="Ch1.S3.SS3">
  <label>3.3</label><title>Extreme biomass burning smoke AOD cases</title>
      <p id="d1e3404">A distinct class of extreme smoke cases comes from pyrocumulonimbus (pyroCb)
events induced by intense biomass burning sources: these events inject smoke
high into the troposphere or even well into the stratosphere (Fromm et al.,
2010; Peterson et al., 2017). A significant pyroCb smoke event that occurred
over British Columbia in August 2017 led to substantial increases in
various optical measures of aerosol concentration in the lower Canadian and
European Arctic (Peterson et al., 2018; Torres et al., 2020; Das et al.,
2021). Ranjbar et al. (2019) showed that a specific 19 August 2017 smoke
event over the high-Arctic PEARL observatory at Eureka, Nunavut, was induced
by the British Colombia pyroCb fires and that it was a statistically significant extreme
FM AOD event. More recent eastern Siberian fires in June–August 2021 induced more than a dozen cases of elevated smoke intrusion into the high
Arctic with some smoke plumes reaching the North Pole and/or its vicinity.
For example, on 5 August 2021, operational NAAPS (common
chemistry, physics, and BB emission sources with the NAAPS-RA) resolved a
smoke plume north of 80<inline-formula><mml:math id="M127" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N (Fig. 4) with AOD values of 2–3. Smoke
AOD over the source region was also 2 to <inline-formula><mml:math id="M128" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula> with a similar
amplitude to AODs measured at Yakutsk. CALIOP data suggested a 1–6 km high
smoke layer in the source region.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e3428">A 5 August 2021 example of BB smoke intrusion into the high
Arctic from fires originating in eastern Siberia. <bold>(a)</bold> Composite true-color
Terra satellite imagery. The red dots represent satellite-detected fire
hotspots. <bold>(b)</bold> Operational NAAPS smoke AOD analysis at 12:00 Z. <bold>(c)</bold> CALIOP 532 nm
attenuated backscatter coefficient showing the smoke layers around the
source area. The yellow stars in <bold>(a)</bold> and <bold>(b)</bold> represent the location of
Yakutsk, which experienced a daily mean total AOD (500 nm) of 2.0 (FM AOD
<inline-formula><mml:math id="M129" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1.9</mml:mn></mml:mrow></mml:math></inline-formula>) and an intra-day peak around 2.5 based on AERONET
V3L1.5 data. Sources: MODIS-Terra true-color satellite imagery and
CALIOP-CALIPSO 532 nm attenuated backscatter coefficient profile
(respectively, <uri>https://worldview.earthdata.nasa.gov/</uri>, last access: 17 July 2022, and
<uri>https://www-calipso.larc.nasa.gov/</uri>, last access: 17 July 2022).</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/9949/2022/acp-22-9949-2022-f04.png"/>

        </fig>

      <p id="d1e3469">Other extreme or near-extreme smoke events in the Arctic have been reported.
A series of intense fires originating in North America led to strong AOD
peaks in the summer of 2015 over Svalbard (Markowicz et al., 2016; Lisok et
al., 2018). Agricultural fires in eastern Europe in the spring of 2006
caused record-high AODs and pollution levels in the European Arctic (Stohl
et al., 2007). The North American boreal fires in the summer of 2004 led to
large-amplitude AOD peaks in Alaska and enhanced AODs on a pan-Arctic scale
(Stohl et al., 2006).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><?xmltex \currentcnt{5}?><?xmltex \def\figurename{Figure}?><label>Figure 5</label><caption><p id="d1e3475">NAAPS-RA daily (550 nm) total-AOD maps at different percentile
levels for the March–August time frame, the maximum AOD, and (rightmost
column) the month that the maximum AOD occurred. The three rows represent,
respectively, the sampling periods of 2003–2019, 2003–2009, and 2010–2019.
The AOD<inline-formula><mml:math id="M130" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> value for 2003–2019 is the same as that of Fig. 1 despite different color scales.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/9949/2022/acp-22-9949-2022-f05.png"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS4">
  <label>3.4</label><title>Geographic distribution of extreme AODs</title>
      <p id="d1e3502">The NAAPS-RA total-AOD map at different percentile levels locally for
March–August 2003–2019 is shown in Fig. 5. We separated the study period
into early (2003–2009) and late (2010–2019) subperiods. The end year of the
first period was chosen as 2009 given the drop in ABF/sulfate emissions due
to the civil Clean Air Acts enacted across the US (e.g., Tosca et al.,
2017; Kaku et al., 2018) as well as Europe and China and the attendant
decrease in ABF/sulfate AOD in these countries/regions (e.g.,
Zhang et al., 2017). This ABF/sulfate AOD decrease was also observed in the
Arctic, as shown in Fig. 13 of Part 1 (Xian et al., 2022). The median Arctic AOD (less than 0.1
as compared with 0.07 for the AERONET sites from Fig. 3 and Table 2) is an
order of magnitude smaller than the maximum AODs. Clear BB smoke features in
the North American and Asian boreal burning regions start to emerge in the
AOD<inline-formula><mml:math id="M131" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> maps (see also Fig. 1). The maximum AOD is high (greater than
2.0) while being relatively low over the Arctic Ocean (<inline-formula><mml:math id="M132" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.3</mml:mn></mml:mrow></mml:math></inline-formula>–1.0) and the North Atlantic, with the lowest values over the generally
high-elevation Greenland landmass. The maximum AOD is associated with peak
burning activities and generally occurs in July and August. The exception is
the Norwegian Sea area, where the maximum AODs occur in March–May. This is
possibly associated with a combined high AOD level from anthropogenic
pollution, marine aerosols, and springtime agriculture fires.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><?xmltex \currentcnt{6}?><?xmltex \def\figurename{Figure}?><label>Figure 6</label><caption><p id="d1e3526">Occurrence of different aerosol species (expressed as a percent)
relative to the occurrence of total-AOD extreme events (daily total AOD <inline-formula><mml:math id="M133" display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> AOD<inline-formula><mml:math id="M134" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> locally) for the March–August time frame. The
sampling periods are the same as in Fig. 5.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/9949/2022/acp-22-9949-2022-f06.png"/>

        </fig>

      <p id="d1e3551">The occurrence of different aerosol species relative to the occurrence of
total AOD for total-AOD extreme events (March–August time frame) are shown
in Fig. 6. The occurrence maps accordingly indicate which aerosol species
are numerically dominant for extreme AOD events. As expected, BB smoke is
the prevailing extreme-event contributor over the North American and Asian
Arctic, especially near the boreal source regions and associated transport
pathways, as well as most of the Arctic Ocean (except the Barents Sea and
the Norwegian Sea). ABF occurrence dominates the low European Arctic.
Sea salt particles and, to a lesser extent, ABF are the most significant
occurrence contributors in the North Atlantic and the Norwegian Sea. Dust
occurrences to extreme AOD events are very small (0 %–10 %) except over the
predominantly high-elevation region of Greenland where the relative
occurrence of high-altitude African dust dominates the relative occurrence
of the other species.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><?xmltex \currentcnt{7}?><?xmltex \def\figurename{Figure}?><label>Figure 7</label><caption><p id="d1e3557">Mean speciated and total AODs averaged for days with speciated AOD
or total AOD <inline-formula><mml:math id="M135" display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> AOD<inline-formula><mml:math id="M136" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> (i.e., the mean value of the top 5 %
AOD data) for the March–August time frame. The sampling periods are the same
as in Figs. 5 and 6.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/9949/2022/acp-22-9949-2022-f07.png"/>

        </fig>

      <p id="d1e3582">In terms of AOD amplitudes for total-AOD extreme events (Fig. 7), BB smoke
AOD shows dominant contributions, especially in the areas near the boreal
source regions and transport pathways, including most areas of the high
Arctic. ABF and sea salt show slightly higher extreme-event AODs than BB
smoke over the North Atlantic and European Arctic. The regional extreme AODs
are not, however, as large as the extreme AODs in the BB smoke-dominant
regions.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8" specific-use="star"><?xmltex \currentcnt{8}?><?xmltex \def\figurename{Figure}?><label>Figure 8</label><caption><p id="d1e3587">Box-and-whisker plot of daily and area-averaged (70–90<inline-formula><mml:math id="M137" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) speciated AOD at 550 nm from NAAPS-RA (2003–2019) for
different months. The box and whiskers represent AOD at the 95th, 90th, 75th, 50th, 25th,
10th, and 5th percentiles. Mean total AODs are shown as solid black circles and
maximum AODs as stars. Maximum AOD values appear as appropriately colored
numerical values if they extend beyond the 0.2 plot maximum.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/9949/2022/acp-22-9949-2022-f08.png"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9" specific-use="star"><?xmltex \currentcnt{9}?><?xmltex \def\figurename{Figure}?><label>Figure 9</label><caption><p id="d1e3607">Seasonal (March to September) time series of daily mean AODs
averaged over the 70–90<inline-formula><mml:math id="M138" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N high-Arctic area for
each individual year of the 2003–2019 period: <bold>(a)</bold> BB smoke AOD and <bold>(b)</bold> total AOD. The years before 2010 are shown as cold colors, and years after
2010 are shown as warm colors. The dashed horizontal lines show the smoke
AOD<inline-formula><mml:math id="M139" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> value of 0.06 and the total-AOD<inline-formula><mml:math id="M140" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> value of 0.14 during the study period.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/9949/2022/acp-22-9949-2022-f09.png"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS5">
  <label>3.5</label><title>Seasonality of extreme AOD events</title>
      <p id="d1e3657">The NAAPS-RA seasonal cycle of total and speciated AOD is shown in Fig. 8
for daily averages across the area north of 70<inline-formula><mml:math id="M141" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N (a latitude
limit which largely excludes BB source regions). The seasonal cycle of
monthly mean total AOD shows relatively higher values in March–April–May (MAM)
compared with the lower AODs in June–July–August (JJA) and a minimum in June.
The spread of the ABF AOD seasonal values is moderately stable, with a
relatively higher mean and median in MAM than JJA. Sea salt AOD and its spread are relatively higher
in the earlier months (March and April). Dust AOD and spread are generally
stable through the season, with a visibly higher mean and median in April and
May. Smoke AOD amplitude and spread exhibit the greatest inter-species
seasonal variations with the lowest mean and spread in March, increased
means and spreads in April, and significantly higher mean and spread in
later months. July and August appear to have the largest mean, spread, and
maximum smoke AODs (a smoke importance statement that is generally
consistent with the results of Fig. 6). These smoke features significantly
contribute to the seasonality of total-AOD extremes. It is also noted that
the MAM total and smoke AOD means approximately equal their medians but
that the JJA means are greater than their medians (and that this is
especially true for August). The greater number of smoke AOD extremes in the
later season and the attendant consequence of greater positive histogram
skewness would explain those relative increases in the mean.</p>
</sec>
<sec id="Ch1.S3.SS6">
  <label>3.6</label><title>Trends of extreme AOD events</title>
      <p id="d1e3677">There is, as shown in Part 1 of the study, a multi-year decreasing MAM trend
and an increasing JJA trend for total AOD in the Arctic over the 2003–2019
sampling period. This was attributed to an overall decrease in MAM and JJA
sulfate/ABF AOD coupled with a negative trend in MAM and a strong positive
trend in JJA for biomass burning smoke AOD. In terms of extreme-event
trends, AOD<inline-formula><mml:math id="M142" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> (Fig. 5) and the average AOD above AOD<inline-formula><mml:math id="M143" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> (Fig. 6)
generally increased over the boreal continents from the 2003–2009 to
2010–2019 period (with the notable exception of Alaska and northeastern
Siberia in 2010–2019). This is consistent with the positive BB emission
trends in JJA north of 50 and 60<inline-formula><mml:math id="M144" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N (for which the
JJA trend dominated the MAM trend inasmuch as JJA was associated with much
higher BB emissions; Part 1).</p>
      <p id="d1e3707">The negligible or slight decrease in high-Arctic AOD<inline-formula><mml:math id="M145" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">50</mml:mn></mml:msub></mml:math></inline-formula>, AOD<inline-formula><mml:math id="M146" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">75</mml:mn></mml:msub></mml:math></inline-formula>, and
AOD<inline-formula><mml:math id="M147" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> values from the 2003–2009 to the 2010–2019 period (Fig. 5) is
likely associated with the generally weak ABF decrease seen in Fig. 7.
However, the increase in the maximum AOD value (Fig. 5) and the contribution
of BB smoke to AOD extreme events (Fig. 7) in the latter period is an
indication of stronger extreme BB smoke influence in more recent years. It
is also noted that the maximum high-Arctic AOD occurred later in the season
(mostly August) in 2010–2019 compared with the more balanced variation
occurring in March through August in 2003–2009. This is likely attributable
to overall lower ABF levels in the 2010–2019 period (especially in MAM) and
a shift in extreme smoke events to later in the season (see discussion below).</p>
      <p id="d1e3737">The time series of high-Arctic-averaged daily mean BB smoke and total AOD
from March to September for all years between 2003–2019 is shown in Fig. 9.
The extreme total-AOD variation is largely dictated by BB smoke. There is
also a discernible 2003–2009 to 2010–2019 springtime reduction in extreme
total AOD: this, as discussed in the previous paragraph, is likely due to an
overall reduction in ABF AOD. The occurrence of extreme smoke events tended
to be more equally distributed over all months (April–August) during the
2003–2009 period while being more concentrated in the late season
(July–August) during the 2010–2019 period. The extreme smoke and total-AOD
trends resembled the extreme smoke occurrence trends: more seasonally
balanced during the 2003–2009 period and summertime dominance during the
2010–2019 period. Specific counts of extreme BB smoke days for different months and years and yearly cumulative extreme AODs also support the seasonal shift of extreme smoke events (Table S1).</p>
      <p id="d1e3740">The occurrence of extreme high-Arctic smoke events thus demonstrates a clear
smoke and total-AOD shift from a more balanced spring and summer to the late
season (notably the months of July and August; see also Table S1). This is
consistent with the temporal shift of fire activity to a later time in
Siberia over 2003–2018 (Liu et al., 2021) and the projection of emerging
pan-Arctic fire regimes marked by increases in the likelihood of extreme
fires later in the growing season (McCarty et al., 2021). An earlier fire
season in the boreal region normally suggests a better-managed forest/land
with fewer large and destructive fires, while a later fire season indicates
the opposite.</p>
      <p id="d1e3744">The shift of boreal fire activity, and the resulting BB smoke AOD extremes
in the Arctic from early season to late season, is probably related to
early-season strengthening of agriculture burning regulations and increased
summertime lightning frequencies with climate change in the latter decade.
For example, the springtime BB smoke AOD peak values in 2003, 2006, and 2008
are all associated with agricultural activity (resulting in fires burning
out of control) and widespread high-latitude burning (Korontzi et al., 2006;
Stohl et al., 2007; Saha et al., 2010). At the same time, with climate
change, lightning activity, and lightning-caused wildfires in summertime
high-latitude regions were observed to increase in the past 2 decades
(Zhang et al., 2021; Bieniek et al., 2020; Coogan et al., 2020). Also noted
is a lengthening of growing season in boreal regions, which implies a lengthening of fire season as well (Park et al., 2016). These factors aside,
climate oscillations, including the Arctic Oscillation, Niño–Southern Oscillation (ENSO), and Pacific
Decadal Oscillation, also affect boreal fire activities (Balzter et al.,
2007; Macias Fauria and Johnson, 2006; Kim et al., 2020). These climate
factors modulate interannual variations and possibly the transport dynamics
of pollutants from the midlatitudes to the Arctic region (e.g., Eckhardt et
al., 2003; Fisher et al., 2010).</p>
      <p id="d1e3747">The dominant contributor, ABF, to regional extreme AOD occurrence and
magnitude in the lower European Arctic decreased slightly from 2003–2009 to
2010–2019 (Figs. 6 and 7): this observation is generally coherent with the
Part 1 results showing a pan-Arctic ABF AOD decrease in the 2003–2019 period
and Fig. 9. Extreme total-AOD events dominated by sea salt contributions in
the North Atlantic and Norwegian Sea increased slightly in 2010–2019. This
was possibly due to the observed increase in cyclonic activities (Rinke et
al., 2017; Waseda et al., 2021; Valkonen et al., 2021). Although the model
simulation of CM AOD is not as skillful as that of FM, trend analysis of CM
AOD which is based on relative change is arguably significant.</p>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <label>4</label><title>Summary</title>
      <p id="d1e3759">AOD data from the NAAPS-RA, the ground-based AERONET, and MAN were employed
in analyzing the 2003–2019 statistics and trends of extreme Arctic AOD
events for spring and summer seasons. Extreme AODs are defined as any AOD
greater than the 95th percentile (AOD<inline-formula><mml:math id="M148" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula>) for any given distribution of
AODs, whether that distribution is generated by the ensemble of AODs
representing the time series of a specific location or of a regional
average. Total, FM, and CM AODs at 550 nm from 6 h resolution NAAPS-RA were
first validated against AERONET and MAN AOD data. NAAPS-RA was shown to be
capable of largely capturing FM and total-AOD ranges and variability. The
NAAPS-RA performance in simulating CM AOD was significantly better if the
temporal resolution of the all-season statistics was less sensitive to high-frequency dust and sea salt events (i.e., the use of temporal resolution bins
of a month rather than 6 h). Statistics of the 6 h Arctic AOD and extreme
AOD events were analyzed. Finally, trends of extreme AOD in the Arctic were
presented and analyzed.</p>
      <p id="d1e3771"><italic>Baseline statistics for 6-hourly AOD</italic>. The median of 6 h total AODs at 550 nm for all Arctic AERONET sites and
MAN retrievals over the 2003–2019 period is 0.07, while AOD<inline-formula><mml:math id="M149" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> is 0.24.
Both the median and AOD<inline-formula><mml:math id="M150" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> values show a dominant FM AOD contribution.
The CM AOD median is 0.01, while AOD<inline-formula><mml:math id="M151" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> is 0.07. The maximum AOD over the
2003–2019 period varies between 0.5–3.0 for measurements made away from BB
source regions and 1.5 to greater than 3.0 for measurements made closer to
BB source regions. The seasonal NAAPS-RA spread of smoke AOD is much higher
than other speciated AODs, including ABF, dust, and sea salt AODs, for all
months between May and August; the spread is especially large in July and
August. These late-season smoke features significantly contribute to the
seasonality and interannual variabilities of extremes in total AOD.</p>
      <p id="d1e3803"><italic>Extreme AOD events</italic>. Extreme AOD events using the Arctic spring and summer data are largely attributable to FM AOD events and notably BB smoke transport events in
general. Extreme Arctic AOD events show large seasonal and interannual
variability, with the interannual AOD variability largely modulated by BB
smoke. Extreme AOD occurrences in the North American Arctic, the Asian
Arctic, and the high Arctic are dominated by BB smoke events. The occurrence
of regionally extreme AOD events is attributed more to ABF in the lower
European Arctic. The extreme-event occurrence dominance of sea salt aerosols
is largely limited to the North Atlantic and Norwegian Sea. The extreme AOD
amplitudes of ABF and sea salt AOD are, however, significantly lower than
those regions where smoke AOD is dominant. Even for sites
distant from BB source regions, BB smoke is the principal driver of AOD
variation above the AOD<inline-formula><mml:math id="M152" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">95</mml:mn></mml:msub></mml:math></inline-formula> threshold.</p>
      <p id="d1e3817"><italic>Shift of extreme AOD events from spring–summer to summer season</italic>. There is an overall increase in the maximum AOD values in the high Arctic
in 2010–2019 compared to 2003–2009, suggesting stronger extreme BB smoke
influence for more recent years. Extreme AOD events are observed to occur in
a more balanced fashion over the entire April–August season during 2003–2009
while being more concentrated in the latter part of the season (i.e., July
and August) during 2010–2019. The seasonal shift in extreme smoke AOD events
is consistent with the multi-year negative MAM trend and positive JJA trend
in BB emissions (north of 50<inline-formula><mml:math id="M153" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, Part 1). These trends are likely
attributable to early season agricultural burning controls and increased
lightning activity and lightning-caused wildfires in summertime in the
boreal high-latitude regions on top of the overall lower level, especially
in spring, of 2010–2019 vs. 2003–2009 anthropogenic aerosols. The shift in
extreme smoke events is consistent with a general multi-year decreasing
springtime trend and an increasing summertime trend of BB emissions north of
50<inline-formula><mml:math id="M154" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N (Part 1, Xian et al., 2022).</p>
      <p id="d1e3841">Global warming is expected to continue generating drier conditions and
increased wildfire activities in the high latitudes (McCarty et al., 2021)
and thus render the Arctic more susceptible to extreme smoke events. These
events can significantly change the regional aerosol budget by bringing
large amounts of smoke aerosols into the Arctic. These extreme smoke events
will likely play an increasingly important Arctic aerosol budget role given
the decreasing (Part 1) baseline in anthropogenic pollution aerosols over
the 2003–2019 period. Smoke aerosols are, notably, much more light-absorbing
than anthropogenic sulfate. Also, their different physical and chemical
properties relative to anthropogenic aerosols will translate into different
efficiencies in their role as CCN and INP. When deposited on surface snow
and ice, they impact the surface radiative forcing budget by reducing
surface albedo. The climate impacts of BB smoke would, accordingly, differ
and possibly counteract the dynamics of anthropogenic aerosols. Therefore,
the baseline AOD trends reported in Part 1 and the trends in extreme AOD
events reported here are important in terms of implications for the changing
Arctic climate. The greater sensitivity of Arctic climate to aerosol
forcings relative to other regions of the globe (e.g., Wang et al., 2018),
the impact of the extreme BB smoke events and their interannual variability,
and trends in Arctic climate warrants further exploration. The statistics of
extreme AODs reported here are expected to help in the formulation of
climate sensitivity experiments and improve our knowledge of the relative
importance of aerosol processes compared to other factors of the changing
Arctic climate.</p>
</sec>

      
      </body>
    <back><notes notes-type="codedataavailability"><title>Code and data availability</title>

      <p id="d1e3849">All data supporting the conclusions of this
paper are available through the links provided below.
<list list-type="bullet"><list-item>
      <p id="d1e3854">AERONET Version 3 Level 2 data: <uri>http://aeronet.gsfc.nasa.gov</uri> (Giles, 2022a)</p></list-item><list-item>
      <p id="d1e3861">MAN data: <uri>https://aeronet.gsfc.nasa.gov/new_web/maritime_aerosol_network.html</uri> (Giles, 2022b)</p></list-item><list-item>
      <p id="d1e3868">NAAPS RA AOD: <uri>https://usgodae.org//cgi-bin/datalist.pl?dset=nrl_naaps_reanalysis&amp;summary=Go</uri> (GODAE, 2022).</p></list-item></list></p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d1e3874">The supplement related to this article is available online at: <inline-supplementary-material xlink:href="https://doi.org/10.5194/acp-22-9949-2022-supplement" xlink:title="pdf">https://doi.org/10.5194/acp-22-9949-2022-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e3883">PX designed this study, performed most of the data
analysis, and wrote the initial paper. All authors contributed to
scientific discussion, revision, and editing of the paper.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e3889">The contact author has declared that none of the authors has any competing interests.</p>
  </notes><notes notes-type="disclaimer"><title>Disclaimer</title>

      <p id="d1e3895">Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e3901">We thank the NASA AERONET and MAN and Environment and Climate change
Canada (ECCC) AEROCAN group for the sun photometer data. We acknowledge the
use of imagery from the NASA Worldview application (<uri>https://worldview.earthdata.nasa.gov</uri>, last access: 17 July 2022) and the NASA
CALIPSO website (<uri>https://www-calipso.larc.nasa.gov/</uri>, last access: 17 July 2022).</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e3912">The authors acknowledge support from NASA's Interdisciplinary Science (IDS)
program (grant no. 80NSSC20K1260), NASA's Modeling, Analysis and Prediction
(MAP) program (grant no. NNX17AG52G), and the Office of Naval Research Code 322. Norm T. O'Neill
and Keyvan Ranjbar's work was supported by the Canadian Space Agency, SACIA-2 project, ref. no. 21SUASACOA, ESS-DA program.</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e3918">This paper was edited by Hailong Wang and reviewed by two anonymous referees.</p>
  </notes><ref-list>
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