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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-21-16593-2021</article-id><title-group><article-title>Influence of springtime atmospheric circulation types on the distribution of air pollutants in the Arctic</article-title><alt-title>Influence of springtime atmospheric circulation types</alt-title>
      </title-group><?xmltex \runningtitle{Influence of springtime atmospheric circulation types}?><?xmltex \runningauthor{M. A. Thomas et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Thomas</surname><given-names>Manu Anna</given-names></name>
          <email>manu.thomas@smhi.se</email>
        <ext-link>https://orcid.org/0000-0002-5709-7507</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Devasthale</surname><given-names>Abhay</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-6717-8343</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Nygård</surname><given-names>Tiina</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-7695-456X</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Research and Development, Swedish Meteorological and Hydrological
Institute (SMHI), Folkborgsvägen 17, <?xmltex \hack{\break}?>Norrköping, 60176, Sweden</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Polar Meteorology and Climatology Group, Finnish Meteorological
Institute (FMI), P.O. Box 503, <?xmltex \hack{\break}?>00101 Helsinki, Finland</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Manu Anna Thomas (manu.thomas@smhi.se)</corresp></author-notes><pub-date><day>12</day><month>November</month><year>2021</year></pub-date>
      
      <volume>21</volume>
      <issue>21</issue>
      <fpage>16593</fpage><lpage>16608</lpage>
      <history>
        <date date-type="received"><day>1</day><month>June</month><year>2021</year></date>
           <date date-type="rev-request"><day>11</day><month>June</month><year>2021</year></date>
           <date date-type="rev-recd"><day>11</day><month>October</month><year>2021</year></date>
           <date date-type="accepted"><day>11</day><month>October</month><year>2021</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2021 </copyright-statement>
        <copyright-year>2021</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="d1e109">The transport and distribution of short-lived climate forcers in
the Arctic are influenced by the prevailing atmospheric circulation patterns.
Understanding the coupling between pollutant distribution and dominant
atmospheric circulation types is therefore important, not least to
understand the processes governing the local processing of pollutants in the Arctic, but also to test the fidelity of chemistry transport models to
simulate the transport from the southerly latitudes. Here, we use a
combination of satellite-based and reanalysis datasets spanning over 12 years (2007–2018) and investigate the concentrations of NO<inline-formula><mml:math id="M1" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, O<inline-formula><mml:math id="M2" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>, CO and aerosols and their co-variability during eight different atmospheric circulation types in the spring season (March, April and May) over the Arctic. We carried out a self-organizing map analysis of mean sea level pressure to derive these circulation types. Although almost all pollutants investigated here show statistically significant sensitivity to the circulation types, NO<inline-formula><mml:math id="M3" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> exhibits the strongest sensitivity among
them. The circulation types with low-pressure systems located over the
northeast Atlantic show a clear enhancement of NO<inline-formula><mml:math id="M4" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and aerosol optical
depths (AODs) in the European Arctic. The O<inline-formula><mml:math id="M5" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations are,
however, decreased. The free tropospheric CO is increased over the Arctic
during such events. The circulation types with atmospheric blocking over
Greenland and northern Scandinavia show the opposite signal in which the
NO<inline-formula><mml:math id="M6" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations are decreased and AODs are smaller than the
climatological values. The O<inline-formula><mml:math id="M7" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations are, however, increased,
and the free tropospheric CO is decreased during such events.</p>

      <p id="d1e176">The study provides the most comprehensive assessment so far of the
sensitivity of springtime pollutant distribution to the atmospheric
circulation types in the Arctic and also provides an observational basis for the evaluation of chemistry transport models.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e188">The transport of anthropogenic pollutants from the southerly latitudes has
many implications for the Arctic (Law and Stohl, 2007; Quinn et al., 2008;
Shindell et al., 2008; Arnold et al., 2016; Willis et al., 2018; Abbatt et
al., 2019; Schmale et al., 2021). At daily to weekly scales, the pollutants
could exert an impact on the direct radiative forcing, thereby conditioning
the atmospheric thermodynamics and influencing the surface energy budget.
The transport of short-lived climate forcers (SLCFs), in particular,
absorbing aerosols such as black carbon, is important in this context. The
SLCFs can modulate the energy budget at shorter timescales, thereby
possibly influencing the seasonal sea-ice evolution. Apart from their direct
radiative effects, the SLCFs and other anthropogenic pollutants can also
influence the cloud properties, exerting so-called indirect effects. At
climate timescales, while mitigating the effects of increased carbon
dioxide (CO<inline-formula><mml:math id="M8" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>) and methane (CH<inline-formula><mml:math id="M9" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:math></inline-formula>) could take many decades to even a few hundred years, the regulation of SLCFs is considered as one of the effective
strategies that could meanwhile be implemented to curb the overall impact of
increasing greenhouse gases.</p>
      <?pagebreak page16594?><p id="d1e209">The Arctic Ocean is a very special region in this context, not only due to
its geography and unique nature of environmental conditions but also due
to the absence of any major sources of anthropogenic pollution in the
central Arctic. The pollution sources are located either in the coastal
zones or in the midlatitude regions. This means that the net effect of
SLCFs and the efficacy of their reduction measures depend heavily on the
atmospheric transport and the prevailing local atmospheric circulation
patterns, which could either dampen or favor the intended effects. This is
also an area of research, where there exists a large knowledge gap
currently. The uncertainties in model simulations of the impact of SLCFs on
the Arctic are therefore high, limiting the design and assessment of the
relevant reduction policies.</p>
      <p id="d1e212">Pollutant transport to the Arctic occurs nearly all year round, and this
transport is heavily influenced by large-scale atmospheric circulation and
various dynamical mechanisms, for example, cyclones, location of the storm
track, high-latitude blockings, and North Atlantic and Arctic oscillations
(Duncan and Bey, 2004; Messori et al., 2018; Papritz and Dunn-Sigouin, 2020),
as well as the local environmental and meteorological conditions (for
example, structure of the atmospheric boundary layer, temperature and
humidity inversions, the state of the sea-ice, clouds) during different
times of the year. In spring, the meteorological conditions in the Arctic
are also usually more diverse than in the winter or the summer months, and
the photochemistry begins to play an important role as the solar
illumination conditions improve. The polar dome (Bozem et al., 2019),
isolating cold air masses in the lower troposphere in the high Arctic from
the rest of the Arctic, starts to weaken in spring, allowing for more
frequent exchange of air masses between the high Arctic and the lower
latitudes. In addition to other anthropogenic sources, the pollutants from
biomass burning are also being carried to the Arctic in spring (Stohl et
al., 2007; Warneke et al., 2009, 2010). A host of studies have rightfully
pointed out the existence, implications and importance of Arctic haze in
shaping the Arctic weather and climate in the springtime. Hence, the spring
season is a good test bed to investigate the coupling of prevailing weather
states and the pollutant distribution in the Arctic. Furthermore, purely
from the observational perspective, the availability of satellite-based
observations from the sensors that rely on the solar channels increases in
spring, as the improved solar illumination conditions allow the retrievals
of trace gases.</p>
      <p id="d1e215">In light of the reasons mentioned above, it is understandable that a number
of major campaigns have been carried out in spring, providing valuable data
and characterizing pollutant variability in relation to the transport and
local meteorological conditions. The aircraft measurements, ARCTAS (Arctic
Research of the Composition of the Troposphere from Aircraft and Satellites)
and ARCPAC (Aerosol, Radiation, and Cloud Processes affecting Arctic
Climate), among others, that were carried out as part of the POLARCAT (Polar
Study using Aircraft, Remote Sensing, Surface Measurements and Models, of
Climate, Chemistry, Aerosols and Transport) campaign for the spring and
summer of 2008, provided a wealth of knowledge on Arctic pollution, the
transport pathways and climate impacts (Law et al., 2014). This campaign
period coincided with a variety of meteorological conditions that affected
the transport of different pollutants into the Arctic. For example, ARCTAS
data constrained with AIRS CO observations revealed that Arctic pollutants
were dominated by European anthropogenic sources from the surface to the free
troposphere in some cases and by Asian anthropogenic sources above 2 km
(Fisher et al., 2010, Jacob et al., 2010). The Asian transport pathways are
mainly via the warm conveyor belts (Stohl, 2006). Low-altitude ARCPAC
flights also revealed increased pollutant concentrations, such as BC,
throughout the Arctic atmospheric column during early spring of 2008,
indicating accumulation of pollutants during the winter months due to lower
temperatures, lack of solar radiation and stable stratification (Spackman et
al., 2010). Also, Warneke et al. (2009) identified a significant influx of
pollutants into Alaska from the forest fires in Russia and the agricultural
burning in Asia. Modeling studies that followed these measurements
estimated a reduction (0.8 % in spring) in snow albedo over the Arctic
owing to BC deposition originating from Russian fires (Wang et al., 2011).</p>
      <p id="d1e219">The large-scale descent and stratospheric intrusions also play a role in the
observed enhancement of pollutants. For example, BrO concentrations at lower
levels were also noted to be enhanced as a result of intrusions of lower
stratospheric air into the troposphere (Jacob et al., 2010). The enhanced
BrO is also closely linked to frontal lifting in a polar cyclone in spring
(Blechschmidt et al., 2016). Despite a negative El Niño–Southern Oscillation (ENSO) year, Arctic weather
was strongly influenced by the Eurasian or North American anthropogenic or
boreal fires (Brock et al., 2011; McNaughton et al., 2011), resulting in
increased concentrations of CO and aerosol loading (van der Werf et al.,
2010; de Villiers et al., 2010; Schmale et al., 2011; Quennehen et al., 2011;
di Pierro et al., 2013). Based on the aircraft measurements, Wespes et al., (2012) inferred that up to respectively 45 % and 60 % of the total O<inline-formula><mml:math id="M10" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and HNO<inline-formula><mml:math id="M11" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> observed below 400 hPa over the Arctic were of
European origin, which is transported via northward and westerly
trans-Siberian pathways. The contribution of these pollutants from the Asian
and North American sectors to the Arctic was much weaker. Most recently,
Thomas et al. (2019) investigated the dependency of aerosol vertical
distribution on the degree of atmospheric stability in the Arctic during
winter and spring using the satellite observations. They argued that the
observed dependency can be explained by the dominance of pollution transport
within the boundary layer during winter and in the free troposphere during
spring.</p>
      <p id="d1e240">It is evident from the previous studies that a detailed assessment of the
co-variability of atmospheric circulation types and pollutants is needed in
the Arctic (a) to fully grasp the coupling between local meteorology,
pollutant distribution and long-range transport in the Arctic and (b) to
improve the representation of such co-variability and coupling in the
models. Such an assessment will also help to evaluate and better constrain the
existing chemistry transport models as well as fully coupled Earth system
models. In the present study, we therefore pose and seek answers to the
following scientific questions.
<list list-type="order"><list-item>
      <p id="d1e245">Which typical atmospheric circulation types (CTs) prevail in the Arctic
during springtime, and what are the typical meteorological conditions
associated with them?</p></list-item><list-item>
      <p id="d1e249">How do these circulation types influence the distribution of trace gases
such as NO<inline-formula><mml:math id="M12" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, O<inline-formula><mml:math id="M13" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and CO?</p></list-item><list-item>
      <p id="d1e271">Is there a distinguishable signal in the aerosol distribution during these
circulation types?</p></list-item></list></p>
</sec>
<?pagebreak page16595?><sec id="Ch1.S2">
  <label>2</label><title>Observational datasets and methodology</title>
      <p id="d1e282">The satellite-based datasets of NO<inline-formula><mml:math id="M14" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, CO and aerosols for March, April
and May months from 2007 to 2018 are analyzed in this study. These are
respectively based on retrievals from the Ozone Monitoring Instrument (OMI)
on board the NASA Aura satellite, the hyperspectral Atmospheric Infrared
Sounder (AIRS) instrument on board the Aqua satellite, and the Cloud and
Aerosol Lidar with Orthogonal Polarization instrument on board the CALIPSO
satellite. All three satellites belong to NASA's Afternoon Train (A-Train)
convoy of satellites, thus providing simultaneous observations in space and
time. The ozone dataset is obtained from the Copernicus Atmospheric
Monitoring Service (CAMS) reanalysis.</p>
      <p id="d1e294">We analyzed the AIRS Standard Daily IR-Only Version 7 product for the 500 hPa CO
retrievals and OMI OMNO2d Version 3 product for the total column NO<inline-formula><mml:math id="M15" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>
retrievals. The surface conditions and cloud cover play an important role in
data sampling. These issues are taken into account before applying
criteria for the selection of the data for each of these species and aerosol optical depth (AOD). In
this study, the all-sky OMI NO<inline-formula><mml:math id="M16" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> retrievals are used, and the quality control is applied similarly to the previous studies (e.g., Thomas and Devasthale, 2017). A sensitivity study, wherein we investigated the NO<inline-formula><mml:math id="M17" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> anomalies during all-sky and clear-sky conditions (not shown here), is carried out.
Though there are some differences in the magnitude of the anomalies, the
overall NO<inline-formula><mml:math id="M18" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> response and patterns remain robust. In the case of CO, the
hyperspectral capability of AIRS allows relatively accurate retrievals even
under the presence of partial cloudiness. Therefore, in this study, we have
considered cloud cover up to 70 %. The high-latitude regions are often
characterized by the presence of either low-level boundary layer clouds or
the high, thin cirrus clouds, both of which do not significantly affect the
AIRS retrievals in the free troposphere at 500 hPa. It is also worth
pointing out that previous studies have shown that the circulation patterns
that favor pollution transport into the Arctic are also associated with the
transport of heat and moisture into the Arctic, which in turn leads to
increased cloudiness (Devasthale et al., 2020; Thomas et al., 2019;
Johansson et al., 2017). Hence, to capture these most realistic scenarios,
stringent thresholds on cloud cover are relaxed in the analysis. Imposing
a strict threshold on cloud cover (for example, analyzing only clear-sky
conditions to ensure the best quality retrievals) would introduce
unrealistic clear-sky biases. To investigate the tropospheric aerosol
optical depths (AODs), the CALIPSO Level 2 standard aerosol profile product
version 4.2 available at 5 km horizontal resolution is used
(CAL_LID_L2_05kmAPro-Standard-V4-20). In the case of the CALIPSO APro product, we select
data only when the cloud–aerosol discrimination score is between and equal
to (<inline-formula><mml:math id="M19" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>50, <inline-formula><mml:math id="M20" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>100) and when the extinction quality flag is 0, 1 or 2. For all
satellite products, the data from the ascending passes (daytime conditions)
are used. We analyze the retrievals designated TqJ (joint temperature and
humidity retrievals) in the AIRS product as they are of the best quality and are
suitable for process and climate studies. These datasets have been
previously used to study the meteorological conditions and pollution
variability in the high-latitude regions, including the Arctic (Devasthale
et al., 2011; Devasthale and Thomas, 2012; Thomas and Devasthale, 2014;
Devasthale et al., 2016; Thomas and Devasthale, 2017; Thomas et al., 2019).</p>
      <p id="d1e348">Furthermore, we analyzed O<inline-formula><mml:math id="M21" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> at 925 hPa from CAMS since the focus is on
the near-surface O<inline-formula><mml:math id="M22" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and also since the satellite-based observations of
the lower tropospheric ozone are either not reliable or available. The
validation of the ozone CAMS reanalysis product is carried out extensively
using ground-based measurements (TOAR database for surface ozone (Schulz et
al., 2017a, b) and ozonesondes globally (Inness et al., 2019; Huijnen et al., 2020). The CAMS assimilation system makes use of data from SCIAMACHY,
MIPAS, OMI, MLS, GOME-2 and SBUV/2 for O<inline-formula><mml:math id="M23" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>. Even though the surface
ozone is primarily model based, upgrades in the CAMS chemical data
assimilation system, assimilated measurements, etc. have improved the near-surface estimates.</p>
      <p id="d1e378">The dominant CTs in the Arctic in spring are identified and clustered by
applying the self-organizing map (SOM) method, developed by Kohonen (2001).
The SOM method uses unsupervised learning to determine generalized patterns
in input data, and the method has previously been utilized to statistically
cluster synoptic weather patterns (e.g., Hewitson and Crane, 2002; Cassano et
al., 2006; Gibson et al., 2017; Nygård et al., 2019). In this study, we
allocate 20 characteristic atmospheric circulation types in spring (MAM,
2007–2018), using mean sea-level pressure (MSLP) data of ERA5 reanalysis
(Copernicus Climate Change Service, 2017) produced by the European Centre
for Medium-Range Weather Forecasts at 6 h intervals as the input data. MSLP
is used here as it is a robust indicator of the atmospheric state in the
Arctic and captures and represents the circulation and flow patterns that
affect the lower troposphere (Neal et al., 2016, and the references therein).
This is important for<?pagebreak page16596?> analyzing the pollution transport processes that occur
mostly in the lower troposphere and their subsequent impacts. In the initial
phase of the SOM analysis, each of the 20 nodes in the SOM array has an
associated reference vector with an equal dimension to the input MSLP data.
Then, each time step of input MSLP data is compared with the reference
vector of each node during the SOM training. The reference vectors, which
are most similar to the input data vector, are adjusted towards the input
data vector. This procedure is repeated until the reference vectors do not
change anymore. The subsequent output is a two-dimensional SOM array of
gridded MSLP fields, having probability density of the input MSLP data. This
array is organized according to similarities in CTs, having the most similar
circulation patterns located next to each other and the most dissimilar
patterns in the corners of the array. Each time step of the input MSLP data
is linked to the most similar circulation type or weather state (node) in
the array. Based on these time steps, we are also able to form composites of
trace gases in each CT separately. Although we originally investigated 20 CTs, here we present the results for eight of those 20 CTs for the sake of
brevity. The selection of these eight CTs is based on (1) the strength of the
signal observed in the trace gases, (2) the frequency of occurrence of the
circulation types and (3) the diversity of the CTs. The results for all 20 CTs are in Appendix A for interested readers. The eight CTs (CT1–CT8)
selected in this study (shown in Fig. 2) correspond respectively to CT1,
CT4, CT9, CT12, CT14, CT18, CT19 and CT20 in Fig. A1 in Appendix A.</p>
      <p id="d1e382">After deriving the prevalent circulation types, the climatological means of
NO<inline-formula><mml:math id="M24" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, CO, O<inline-formula><mml:math id="M25" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and AOD during the March, April and May months are
computed separately. For each circulation type, the number of days that
represent that type could be different in each month. In order to compute a
climatological mean that takes into account this difference, we weighed the
climatological means of each month with weighing factors shown in Fig. 1,
giving climatological means of NO<inline-formula><mml:math id="M26" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, CO, O<inline-formula><mml:math id="M27" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and AOD associated with
each weather state. The composites of NO<inline-formula><mml:math id="M28" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, CO, O<inline-formula><mml:math id="M29" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and AOD for each
weather state are then computed. The anomalies shown later are the
differences between these composites and the weighted climatological means
for each weather state. Only those trace-gas anomalies that are
statistically significant using Student's <inline-formula><mml:math id="M30" display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula> test at the 90 % confidence
interval are shown.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><?xmltex \currentcnt{1}?><?xmltex \def\figurename{Figure}?><label>Figure 1</label><caption><p id="d1e449">The number of days analyzed for each circulation type and
month <bold>(a)</bold> and the corresponding weighing factor used to compute the
climatologies of trace gases and aerosols <bold>(b)</bold>.</p></caption>
        <?xmltex \igopts{width=227.622047pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f01.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2" specific-use="star"><?xmltex \currentcnt{2}?><?xmltex \def\figurename{Figure}?><label>Figure 2</label><caption><p id="d1e466">Mean sea level pressure (MSLP) averaged over the cases belonging to
each of the eight circulation types chosen from the 20 circulation types shown
in the Appendix A.</p></caption>
        <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f02.png"/>

      </fig>

</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Overview of the CTs and associated meteorological conditions</title>
      <p id="d1e483">Figure 2 shows the mean MSLP patterns during the eight CTs that are chosen from
the SOM analysis. These types are mainly characterized by different
locations and strengths of cyclones and anticyclones with respect to one
another. For example, the first CT (CT1) is characterized by the most
commonly observed low-pressure regimes in the northeast Atlantic and
European Arctic and an intense Beaufort high on the Pacific side of the
Arctic. In CT2, the low-pressure systems in the Greenland and Norwegian seas
gradually intensify, while the anticyclones move over the Chukchi and East
Siberian seas and weaken in their intensity. In the case of CT3, almost half
of the Arctic (Greenland, Canadian Archipelago and Beaufort Sea and Alaska)
is under the influence of a strong anticyclone, with the center of action
located east–west of the international date line. The strongest anticyclonic
conditions are observed during CT3, while the strongest cyclonic conditions
are observed in CT2 over the Greenland and Norwegian seas. CT4 shows a
tripole pattern wherein strong low-pressure systems are located over the
Barents and Kara seas as well as over Alaska at the opposite side of the
Arctic, while a weaker but noticeable high-pressure zone is observed over
the Canadian archipelago. CT5 is characterized by anticyclonic conditions
dominating over the entire central Arctic as well as Greenland and the
Canadian archipelago. CT6 and CT7 show dipole patterns (with different
intensities) with cyclonic conditions over Siberia and anticyclonic
conditions prevailing at the opposite side of the Arctic Circle. Finally in
CT8, cyclonic conditions are observed in both the northeast Atlantic and
Siberia, while the anticyclonic conditions are observed over Scandinavia and Beaufort
Sea. The SOM analysis presented in Fig. 2 reveals how varied and complex the
atmospheric<?pagebreak page16597?> large-scale circulation patterns can be over the Arctic in
spring.</p>
      <p id="d1e486">Atmospheric circulation drives the transport in the atmosphere. For example,
it largely distributes moisture in the Arctic atmosphere by dictating its
horizontal transport and modulating the local evaporation at the surface.
Figure 3 shows the specific humidity anomalies (d<inline-formula><mml:math id="M31" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula>), based on AIRS data,
associated with those eight CTs. These anomalies are a good indicator (and
manifestation) of the transport patterns shaped by the cyclonic and
anticyclonic conditions mentioned above. Furthermore, atmospheric humidity
has an impact on the aerosol optical properties and morphology as well as on
the processes affecting the lifetime of trace gases. An increase in d<inline-formula><mml:math id="M32" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula> is
detected in the Greenland and Norwegian seas in CT1 and CT2 due to the
cyclonic conditions in the northeast Atlantic transporting more heat and
moisture. In CT3, in the absence of such transport in the northeast Atlantic
and due to the presence of anticyclones over Greenland and the Canadian
Archipelago, drier and cooler air masses are transported over the Greenland,
Norwegian and Barents seas, as seen in the reduction of humidity anomalies
over these areas. A similar decrease in humidity is also observed in CT4 and
CT6 over the Greenland and Norwegian seas. In CT4, an increase in d<inline-formula><mml:math id="M33" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula> can be seen
over the Laptev Sea as a result of the strong low-pressure systems centered
eastward of Scandinavia over the Barents and Kara seas along the Russian
coast. In CT8, a slight increase in humidity is seen over the entire Arctic
Ocean due to the influence of low-pressure systems located over the
northeast Atlantic and northern Siberia. Our results indicate that the CTs
derived based on MSLP can also be used to analyze the free and upper
tropospheric pollutants. The AIRS-derived geopotential height anomalies at
500 hPa are shown in Fig. 4. There is a coupling between the lower and upper
level circulation during those circulation types and, especially, a good
resemblance in the locations of the centers of action of low-pressure
systems and anticyclones derived based on MSLP and the 500 hPa geopotential
heights.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e512">The 850 hPa specific humidity anomalies (g kg<inline-formula><mml:math id="M34" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> based on AIRS data for the eight circulation types.</p></caption>
        <?xmltex \igopts{width=239.00315pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f03.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e539">Geopotential height anomalies (m) at 500 hPa based on AIRS data for
the eight circulation types.</p></caption>
        <?xmltex \igopts{width=239.00315pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f04.png"/>

      </fig>

<?xmltex \hack{\newpage}?>
</sec>
<?pagebreak page16598?><sec id="Ch1.S4">
  <label>4</label><title>Covariability of CTs and air pollutants</title>
      <p id="d1e558">The response of NO<inline-formula><mml:math id="M35" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> to the CTs is shown in Fig. 5 in terms of weighed
anomalies. It is to be noted that, while the SOM analysis is done over the
region northward of 60<inline-formula><mml:math id="M36" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N in order to emphasize the circulation patterns in the Arctic region, we present the anomalies of the pollutants northward of 50<inline-formula><mml:math id="M37" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N in order to provide the large-scale spatial context. It can be seen that the spatial distribution of NO<inline-formula><mml:math id="M38" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> is highly sensitive to the CTs, not only over the polluted mainland and source regions but also over the Arctic
Ocean. Particularly over northern Europe, a distinct pattern emerges,
wherein the NO<inline-formula><mml:math id="M39" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> anomalies change sign gradually from CT1 to CT8 in
response to the changing atmospheric circulation patterns. In CT1 and CT2,
there is a clear transport signal in the NO<inline-formula><mml:math id="M40" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> anomalies. The location
of low-pressure systems in the northeast Atlantic favors the transport of
NO<inline-formula><mml:math id="M41" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> from the northern, central and eastern European regions into the
Arctic. The increased specific humidity anomalies in the European Arctic
further confirm such a transport (Fig. 3). The strongest signal is observed
in CT2, when the center of action of the polar vortex is located over Greenland
(Figs. 2 and 4) and the intensity of the vortex is stronger, favoring the
increased transport of NO<inline-formula><mml:math id="M42" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> in the Barents and Kara seas, reaching even
further north into the Arctic. Previous studies have indicated that, in the
European sector of the Arctic, such transport occurs predominantly in the
lower troposphere (Stohl, 2006; Thomas et al., 2019). A pronounced increase
in humidity anomalies is also seen over these regions in CT2. Among all
circulation types, the highest NO<inline-formula><mml:math id="M43" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> anomalies are observed over
Scandinavia in CT1 and CT2, suggesting a noticeable influence of these
circulation types in the pollution variability in these countries. The
transport from the central and eastern European countries is especially
prominent in CT2. It is to be noted that the circulation types CT1 and CT2
roughly resemble the typical loading patterns of North Atlantic Oscillation
and/or Arctic Oscillations over the central and Eurasian Arctic, which is
shown to have a noticeable impact on the pollutant variability over these
regions (e.g., Eckhardt et al., 2003; Christoudias et al., 2012).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><?xmltex \currentcnt{5}?><?xmltex \def\figurename{Figure}?><label>Figure 5</label><caption><p id="d1e645">NO<inline-formula><mml:math id="M44" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> total column anomalies (molecules cm<inline-formula><mml:math id="M45" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> based on OMI
data for the eight circulation types. Only those anomalies that are
statistically significant at the 90 % confidence level are shown.</p></caption>
        <?xmltex \igopts{width=239.00315pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f05.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6"><?xmltex \currentcnt{6}?><?xmltex \def\figurename{Figure}?><label>Figure 6</label><caption><p id="d1e680">The 925 hPa O<inline-formula><mml:math id="M46" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> anomalies (ppbv) based on CAMS data for the eight
circulation types. Only those anomalies that are statistically significant
at the 90 % confidence level are shown.</p></caption>
        <?xmltex \igopts{width=239.00315pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f06.png"/>

      </fig>

      <p id="d1e699">An entirely opposite NO<inline-formula><mml:math id="M47" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> response is seen in CT5 to CT8. In CT5 and CT6
with anticyclonic conditions prevailing over Greenland and northern north
Atlantic at varying intensity, the transport of cleaner air masses from the
central Arctic leads to negative NO<inline-formula><mml:math id="M48" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> anomalies over the central and
northern parts of Europe. The anticyclone further moves eastwards over
Greenland and Norwegian seas and over northern Scandinavia from CT5 to CT6,
blocking the transport from the southerly latitudes and therefore leading to
negative NO<inline-formula><mml:math id="M49" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> anomalies during these circulation types. In CT7, the
circulation pattern in the Canadian Archipelago and European sector of the
Arctic together with cyclonic conditions in central and eastern Siberian
regions facilitate the northeast Asian transport of NO<inline-formula><mml:math id="M50" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> into Alaska
and northern Canada. In CT8, the low-pressure systems over the northeast
Atlantic and Siberia as well as the Kara and Laptev seas lead to a slight increase in
NO<inline-formula><mml:math id="M51" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentration in the Barents Sea. The blocking over southern
Scandinavia and Europe however limits the large-scale transport into the
Arctic from the European sector. The northeast Asian regions and<?pagebreak page16599?> northern
Pacific Ocean show no sensitivity to the circulation types, most likely due
to the persistent nature of westerly winds over this region in combination
with the persistent continental pollution outflow over the northern Pacific.</p>
      <p id="d1e747">The O<inline-formula><mml:math id="M52" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> anomalies at 925 hPa also show sensitivity to the circulation
types. They appear to be opposite in nature to that of the NO<inline-formula><mml:math id="M53" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>
anomalies. For example, a reduction in the O<inline-formula><mml:math id="M54" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations over
the northeast Atlantic and Scandinavia seen in CT1 and CT2 is consistent with
the strong NO<inline-formula><mml:math id="M55" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> increases observed during the same circulation types. A
statistically significant increase in the central Arctic is seen in CT1 and
CT3. However, the corresponding NO<inline-formula><mml:math id="M56" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> anomalies over the central Arctic
in these circulation types are not statistically significant. An inverse
correspondence between O<inline-formula><mml:math id="M57" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and NO<inline-formula><mml:math id="M58" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> away from the source regions is
not expected due to the different lifetimes, aging and transport processes.
A decrease in O<inline-formula><mml:math id="M59" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations over the central Arctic corresponds to
the presence of cyclonic conditions over Eurasia and Siberia (CT6–CT8).</p>
      <p id="d1e823">The springtime photochemistry in the Arctic is very complex, as duly noted
in the rich literature that documents the research and observations on this
subject matter (Lu et al., 2019, and the references therein). The
interactions between NO<inline-formula><mml:math id="M60" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and O<inline-formula><mml:math id="M61" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> are also highly nonlinear in
reality and hence a one-to-one correlation can not be established. In the
troposphere, NO is converted to NO<inline-formula><mml:math id="M62" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> in the presence of O<inline-formula><mml:math id="M63" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>, which is
a potential sink for O<inline-formula><mml:math id="M64" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>. However, during sunlit conditions, NO<inline-formula><mml:math id="M65" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> is converted back to NO via photolysis, which results in O<inline-formula><mml:math id="M66" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
production. Apart from these chemical reactions, local meteorological
conditions such as temperature, relative humidity and rainfall play an
important role in the production and dispersion of these pollutants.
Stratospheric intrusions are another source of O<inline-formula><mml:math id="M67" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> variability in the
troposphere that may play a role under different circulation types (Yates et
al., 2013; Langford et al., 2015; Lin et al., 2015). The persistent
anticyclonic conditions could not only lead to the accumulation of the
tropospheric O<inline-formula><mml:math id="M68" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> but also favor the large-scale descent or intrusions
into the lower troposphere, leading to positive O<inline-formula><mml:math id="M69" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> anomalies.</p>
      <p id="d1e917">Figure 7 shows the tropospheric AOD anomalies based on the CALIOP-CALIPSO
aerosol profile product. It is to be noted that, being an active profiler,
the spatial coverage of CALIOP-CALIPSO is very poor and the anomalies look
patchy, particularly over the inland regions because of a limited number of
samples for each circulation type. The passive imagers either do not have
AOD data available in spring (due to poor illumination conditions) or the
quality of the retrievals can be very poor due to the challenging surface
conditions and the underlying uncertainties in cloud masking. CALIOP
provides the most accurate sampling of aerosols over the Arctic Ocean in
spring in comparison to passive imagers, but with this trade-off of having
poor spatial sampling, and therefore the AOD data have to be interpreted
cautiously. We, nonetheless, decided to include CALIPSO in the analysis
since it can provide an important context while studying the trace gas
variability. For example, we can see that there are at least two signals
that are robust and consistent with other observations. An increase in AOD
in CT1 and CT2 is observed in the Greenland and Norwegian seas and northern
Scandinavia, which is consistent with the increases in NO<inline-formula><mml:math id="M70" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, further
confirming the role of these circulation types in transporting the
pollutants into the Arctic. An increase in humidity, as mentioned earlier,
in CT1 and CT2 impacts the AODs due to increased water uptake during
transport. These circulation types are similar to those that could change
the stability regimes as a result of heat and moisture transport over the
colder sea-ice surfaces in the inner Arctic and trapping the aerosols and
pollutants below the inversions in the Eurasian sector of the Arctic, as
previously reported in Thomas et al. (2019). The opposite tendencies in CT5
and CT6, wherein the negative AOD anomalies are observed over the Norwegian
Sea and northern Scandinavia, are also consistent with the NO<inline-formula><mml:math id="M71" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>
decreases observed in these circulation types. The anticyclones prevailing
over Greenland and north of Scandinavia block the transport of trace gases
and aerosols into the Arctic during these circulation patterns. The
increased AODs along the western coast of Scandinavia in CT3 could be due to
the location of anticyclones in the Arctic and the low-pressure systems in
central Europe that transport pollutants from eastern Europe and western
parts of Russia, including the biomass burning regions, over these coastal
regions. In the case of other circulation types, the AOD anomalies are too
patchy to draw meaningful conclusions in the sense that there are no
consistent features with either the meteorological conditions or other
pollutants.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7"><?xmltex \currentcnt{7}?><?xmltex \def\figurename{Figure}?><label>Figure 7</label><caption><p id="d1e940">Tropospheric AOD anomalies based on CALIOP-CALIPSO data for the eight
circulation types with 90 % confidence.</p></caption>
        <?xmltex \igopts{width=239.00315pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f07.png"/>

      </fig>

      <p id="d1e950">Unlike tropospheric O<inline-formula><mml:math id="M72" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and NO<inline-formula><mml:math id="M73" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, CO has an atmospheric lifetime
ranging from a few weeks to a few months and therefore is often regarded as a
suitable tracer to study the long-range pollution transport. Due to its
longevity, the spatial distribution of CO in the free troposphere is also
quite homogeneous compared to other trace gases, and the local pollution
variability is often diffused in the large-scale signal. However, CO is an
excellent tracer to study the coupling between the pollution variability in
the free troposphere and the<?pagebreak page16600?> lower tropospheric circulation patterns, given
the influence of these CTs on the entire troposphere, and also to study the
large-scale, first-order impact of the CTs on the free tropospheric
pollutants. Such a large-scale signal is indeed visible in the CO anomalies
shown in Fig. 8. Two main regimes can be seen: one dominated by the
Arctic-wide increases in the CO concentrations (e.g., CT1 to CT2) when the low-pressure systems are active in the North Atlantic and the other when the
decreases in the CO concentrations (e.g., CT5 to CT7) can be seen over much of
the Arctic likely due to the atmospheric blocking over those regions. The CO
anomalies over Scandinavia, the northeast Atlantic, Greenland, and the Norwegian and
Barents seas show the strongest sensitivity to the circulation types.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8"><?xmltex \currentcnt{8}?><?xmltex \def\figurename{Figure}?><label>Figure 8</label><caption><p id="d1e973">The 500 hPa CO anomalies as volume mixing ratios based on AIRS data for
the eight circulation types with 90 % confidence.</p></caption>
        <?xmltex \igopts{width=239.00315pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f08.png"/>

      </fig>

</sec>
<sec id="Ch1.S5" sec-type="conclusions">
  <label>5</label><title>Conclusions</title>
      <p id="d1e991">The transport and the distribution of the pollutants in the Arctic,
especially that of the short-lived climate forcers, depends heavily on the
prevailing atmospheric circulation patterns. Understanding pollutant
variability in relation to the dominant circulation types is therefore
important. Here, we investigate the concentrations of NO<inline-formula><mml:math id="M74" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, O<inline-formula><mml:math id="M75" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>, CO
and aerosols and their co-variability during the eight different circulation
types in the spring season (March, April and May) over the Arctic. The
circulation types discussed in this study are derived by the self-organizing
map analysis of MSLP. A combination of satellite-based and reanalysis
datasets spanning 12 years (2007–2018) is used. The following
conclusions are drawn from the analysis.</p>
      <p id="d1e1012"><list list-type="order">
          <list-item>

      <p id="d1e1017">The eight characteristic circulation patterns during spring, allocated by the
SOM analysis based on the MSLP fields, represent different locations and
intensities of cyclonic and anticyclonic events in relation to each other.
The MSLP circulation patterns are connected to 500 hPa geopotential height
anomalies and also shape the atmospheric humidity distribution. The
circulation patterns largely dictate the transport in the atmosphere,
especially from the main source areas in the southerly latitudes into the
Arctic.</p>
          </list-item>
          <list-item>

      <p id="d1e1023">It is observed that all pollutants investigated here show sensitivity to the
circulation types, and some common patterns emerge in their response.
NO<inline-formula><mml:math id="M76" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> shows the strongest sensitivity among the trace gases and aerosols
analyzed here.</p>
          </list-item>
          <list-item>

      <p id="d1e1038">The circulation types (CT1, CT2) with low-pressure systems located in the
northeast Atlantic show a clear statistically significant enhancement of
NO<inline-formula><mml:math id="M77" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and AOD in the European Arctic. The O<inline-formula><mml:math id="M78" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations are
however decreased in such events.</p>
          </list-item>
          <list-item>

      <p id="d1e1062">The circulation types (CT5, CT6 and CT7) with atmospheric blocking over
Greenland and northern Scandinavia show the opposite signal, in that the
NO<inline-formula><mml:math id="M79" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations are decreased and AODs are smaller than the
climatological values. The O<inline-formula><mml:math id="M80" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations are however increased
during these events in the European Arctic.</p>
          </list-item>
          <list-item>

      <p id="d1e1086">The first-order signal of the influence of circulation types on the free
tropospheric CO is seen, with two main regimes emerging. The first regime
shows the Arctic-wide positive anomalies in the CO concentrations when the
low-pressure systems are active in the North Atlantic and the other when the
negative CO anomalies are observed due to the atmospheric blocking over
those regions.</p>
          </list-item>
        </list></p>
      <p id="d1e1091">The present study provides the most comprehensive investigations so far of
the sensitivity of springtime pollutant distribution to the atmospheric
circulation types in the Arctic, also providing an observational basis for
the evaluation of chemistry transport models.</p><?xmltex \hack{\clearpage}?>
</sec>

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

<?pagebreak page16601?><app id="App1.Ch1.S1">
  <?xmltex \currentcnt{A}?><label>Appendix A</label><title/>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.S1.F9"><?xmltex \currentcnt{A1}?><?xmltex \def\figurename{Figure}?><label>Figure A1</label><caption><p id="d1e1107">Mean sea level pressure (MSLP) averaged over the cases belonging
to each of the 20 circulation types. The chosen eight circulation types are
shown in the brackets.</p></caption>
        <?xmltex \hack{\hsize\textwidth}?>
        <?xmltex \igopts{width=449.553543pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f09.png"/>

      </fig>

<?xmltex \hack{\clearpage}?><?xmltex \floatpos{h!}?><fig id="App1.Ch1.S1.F10"><?xmltex \currentcnt{A2}?><?xmltex \def\figurename{Figure}?><label>Figure A2</label><caption><p id="d1e1121">Specific humidity anomalies (g kg<inline-formula><mml:math id="M81" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) at 850 hPa based on AIRS data
for the 20 circulation types.</p></caption>
        <?xmltex \hack{\hsize\textwidth}?>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f10.png"/>

      </fig>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.S1.F11"><?xmltex \currentcnt{A3}?><?xmltex \def\figurename{Figure}?><label>Figure A3</label><caption><p id="d1e1147">Geopotential height anomalies (m) at 500 hPa based on AIRS data
for the 20 circulation types.</p></caption>
        <?xmltex \hack{\hsize\textwidth}?>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f11.png"/>

      </fig>

<?xmltex \hack{\clearpage}?><?xmltex \floatpos{h!}?><fig id="App1.Ch1.S1.F12"><?xmltex \currentcnt{A4}?><?xmltex \def\figurename{Figure}?><label>Figure A4</label><caption><p id="d1e1161">NO<inline-formula><mml:math id="M82" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> total column anomalies (molecules cm<inline-formula><mml:math id="M83" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> based on OMI
data for the 20 circulation types. Only those anomalies that are
statistically significant at the 90 % confidence level are shown.</p></caption>
        <?xmltex \hack{\hsize\textwidth}?>
        <?xmltex \igopts{width=224.776772pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f12.png"/>

      </fig>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.S1.F13"><?xmltex \currentcnt{A5}?><?xmltex \def\figurename{Figure}?><label>Figure A5</label><caption><p id="d1e1198">The 925 hPa O<inline-formula><mml:math id="M84" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> anomalies as volume mixing ratios based on CAMS
data for the 20 circulation types. Only those anomalies that are
statistically significant at the 90 % confidence level are shown.</p></caption>
        <?xmltex \hack{\hsize\textwidth}?>
        <?xmltex \igopts{width=224.776772pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f13.png"/>

      </fig>

<?xmltex \hack{\clearpage}?><?xmltex \floatpos{h!}?><fig id="App1.Ch1.S1.F14"><?xmltex \currentcnt{A6}?><?xmltex \def\figurename{Figure}?><label>Figure A6</label><caption><p id="d1e1222">Tropospheric AOD anomalies based on CALIOP-CALIPSO data for the
20 circulation types. Only those anomalies that are statistically
significant at the 90 % confidence level are shown.</p></caption>
        <?xmltex \hack{\hsize\textwidth}?>
        <?xmltex \igopts{width=224.776772pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f14.png"/>

      </fig>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.S1.F15"><?xmltex \currentcnt{A7}?><?xmltex \def\figurename{Figure}?><label>Figure A7</label><caption><p id="d1e1235">The 500 hPa CO anomalies as volume mixing ratios based on AIRS data
for the 20 circulation types. Only those anomalies that are statistically
significant at the 90 % confidence level are shown.</p></caption>
        <?xmltex \hack{\hsize\textwidth}?>
        <?xmltex \igopts{width=224.776772pt}?><graphic xlink:href="https://acp.copernicus.org/articles/21/16593/2021/acp-21-16593-2021-f15.png"/>

      </fig>

<?xmltex \hack{\clearpage}?><?xmltex \hack{\newpage}?>
</app>
  </app-group><notes notes-type="dataavailability"><title>Data availability</title>

      <p id="d1e1253">All datasets used in the present study are publicly available as follows.</p>

      <p id="d1e1256">The daily total column NO<inline-formula><mml:math id="M85" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> retrievals (L2) can be accessed at
<ext-link xlink:href="https://doi.org/10.5067/Aura/OMI/DATA2018" ext-link-type="DOI">10.5067/Aura/OMI/DATA2018</ext-link> (Krotkov et al., 2019).</p>

      <p id="d1e1271">The AIRS satellite version 7 dataset is used for the 500 hPa daily CO in this study and can be accessed at the following link: <uri>https://airs.jpl.nasa.gov/data/get-data/standard-data/</uri> (NASA Jet Repulsion Laboratory, 2021a). The data were processed at the Jet Propulsion Laboratory, California Institute of Technology. The details are published at
<uri>https://docserver.gesdisc.eosdis.nasa.gov/public/project/AIRS/Overview_of_the_AIRS_Mission.pdf</uri> (NASA Jet Propulsion Laboratory, 2021b).</p>

      <p id="d1e1280">The near-surface ozone data from the CAMS (Copernicus Atmosphere Monitoring Service) database can be accessed via the following link: (<uri>https://ads.atmosphere.copernicus.eu/cdsapp#!/dataset/cams-global-reanalysis-eac4?tab=overvieware</uri>, Copernicus Atmosphere Monitoring Service, 2021) and are provided by the European Union’s Earth Observation Programme, Copernicus.</p>

      <p id="d1e1286">The CALIPSO Level 2 standard aerosol profile product version 4.2 available at 5 km horizontal resolution is used (CAL_LID_L2_05kmAPro-Standard-V4-20)
for the aerosol optical depths in this study. The data are accessible via
<ext-link xlink:href="https://doi.org/10.5067/CALIOP/CALIPSO/LID_L2_05KMAPRO-STANDARD-V4-20" ext-link-type="DOI">10.5067/CALIOP/CALIPSO/LID_L2_05KMAPRO-STANDARD-V4-20</ext-link> (NASA Earth Data, 2020), created by NASA Langley Atmospheric Science Data Center DAAC.
The mean sea level pressure (MSLP) data are from the ERA5 reanalysis
<ext-link xlink:href="https://doi.org/10.1002/qj.3803" ext-link-type="DOI">10.1002/qj.3803</ext-link> (Hersbach et al., 2020) and are available at the Climate Data Store (CDS) via the link   <uri>https://cds.climate.copernicus.eu/cdsapp#!/dataset/reanalysis-era5-single-levels?tab=overview</uri> (Copernicus Climate Change Service, 2017).</p>
  </notes><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e1301">MAT and AD designed the study. MAT carried out the analysis and wrote the
first draft of the paper. TN performed and provided the SOM analysis.
All authors contributed to the writing and interpretation of the results.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e1307">The contact author has declared that neither they nor their co-authors have any competing interests.</p>
  </notes><notes notes-type="disclaimer"><title>Disclaimer</title>

      <p id="d1e1313">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="d1e1319">The study was funded by the Swedish National Space Agency (grant number
94/16). Tiina Nygård acknowledges the funding by the Academy of Finland via project
TODAy (grant number 308441). The authors would like to thank the OMI, AIRS
and CALIPSO Science Teams for the data products as well as CAMS and ECMWF
for the corresponding reanalysis data products.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e1324">This research has partly been supported by the Swedish National Space Agency (grant no. 94/16) and partly by the Academy of Finland (grant no. 308441).</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e1330">This paper was edited by Bryan N. Duncan and reviewed by two anonymous referees.</p>
  </notes><ref-list>
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