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<article xmlns:xlink="http://www.w3.org/1999/xlink" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:oasis="http://docs.oasis-open.org/ns/oasis-exchange/table" xml:lang="en" dtd-version="3.0" article-type="research-article"><?xmltex \bartext{Research article}?>
  <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-23-4031-2023</article-id><title-group><article-title>Why is ozone in South Korea and the <?xmltex \hack{\break}?> Seoul metropolitan area so high and increasing?</article-title><alt-title>Why is ozone in South Korea and the Seoul metropolitan area so high and increasing?</alt-title>
      </title-group><?xmltex \runningtitle{Why is ozone in South Korea and the Seoul metropolitan area so high and increasing?}?><?xmltex \runningauthor{N. K. Colombi et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Colombi</surname><given-names>Nadia K.</given-names></name>
          <email>ncolombi@g.harvard.edu</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Jacob</surname><given-names>Daniel J.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Yang</surname><given-names>Laura Hyesung</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-0057-7120</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Zhai</surname><given-names>Shixian</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-0073-7809</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3 aff4">
          <name><surname>Shah</surname><given-names>Viral</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-5547-106X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>Grange</surname><given-names>Stuart K.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-4093-3596</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Yantosca</surname><given-names>Robert M.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-3781-1870</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff6">
          <name><surname>Kim</surname><given-names>Soontae</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff7">
          <name><surname>Liao</surname><given-names>Hong</given-names></name>
          
        </contrib>
        <aff id="aff1"><label>1</label><institution>Department of Earth and Planetary Sciences, Harvard University,
Cambridge, MA 02138, USA</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>John A. Paulson School of Engineering and Applied
Sciences, <?xmltex \hack{\break}?> Harvard University, Cambridge, MA 02138, USA</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Global Modeling and Assimilation Office, Goddard Space Flight
Center, NASA, Greenbelt, MD 20771, USA</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Science Systems and Applications, Inc., Lanham, MD 20706, USA</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>Empa, Swiss Federal Laboratories for Materials Science and Technology, <?xmltex \hack{\break}?>
Überlandstrasse 129, 8600 Dübendorf, Switzerland</institution>
        </aff>
        <aff id="aff6"><label>6</label><institution>Department of Environmental and Safety Engineering, Ajou University, <?xmltex \hack{\break}?>
Suwon, Gyeonggi 16499, South Korea</institution>
        </aff>
        <aff id="aff7"><label>7</label><institution>Jiangsu Key Laboratory of Atmospheric Environment Monitoring and
Pollution Control, <?xmltex \hack{\break}?> Jiangsu Collaborative Innovation Center of Atmospheric
Environment and Equipment Technology, <?xmltex \hack{\break}?> School of Environmental Science &amp;
Engineering, <?xmltex \hack{\break}?> Nanjing University of Information Science &amp; Technology,
Nanjing 210044, China</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Nadia K. Colombi (ncolombi@g.harvard.edu)</corresp></author-notes><pub-date><day>5</day><month>April</month><year>2023</year></pub-date>
      
      <volume>23</volume>
      <issue>7</issue>
      <fpage>4031</fpage><lpage>4044</lpage>
      <history>
        <date date-type="received"><day>1</day><month>December</month><year>2022</year></date>
           <date date-type="rev-request"><day>9</day><month>December</month><year>2022</year></date>
           <date date-type="rev-recd"><day>9</day><month>March</month><year>2023</year></date>
           <date date-type="accepted"><day>10</day><month>March</month><year>2023</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2023 </copyright-statement>
        <copyright-year>2023</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="d1e211">Surface ozone pollution in South Korea has increased over
the past 2 decades, despite efforts to decrease emissions, and is
pervasively in exceedance of the maximum daily 8 h average (MDA8) standard
of 60 ppb. Here, we investigate the 2015–2019 trends in surface ozone and
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> concentrations over South Korea and the Seoul metropolitan area (SMA),
focusing on the 90th percentile MDA8 ozone as an air quality metric. We
use a random forest algorithm to remove the effect of meteorological variability
on the 2015–2019 trends and find an ozone increase of up to 1.5 ppb a<inline-formula><mml:math id="M2" 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>
in April–May, while 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> decreases by 22 %.
Global 3-D atmospheric chemistry model simulations including recent chemical updates can successfully simulate surface ozone over South Korea and China as well as the very high free-tropospheric ozone
observed above 2 km altitude (mean 75 ppb in May–June) and can reproduce the observed 2015–2019 emission-driven ozone trend over the SMA including its seasonality.
Further
investigation of the model trend for May, when meteorology-corrected ozone
and its increase are the highest, reveals that a decrease in South Korea NO<inline-formula><mml:math id="M4" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula>
emissions is the main driver for the SMA ozone increase. Although this
result implies that decreasing volatile organic compound (VOC) emissions is
necessary to decrease ozone, we find that ozone would still remain above 80 ppb even if all anthropogenic emissions in South Korea were shut off. China
contributes only 8 ppb to this elevated South Korea background, and ship
emissions contribute only a few parts per billion.
Zeroing out all anthropogenic emissions in East Asia in the model indicates
a remarkably high external background of 56 ppb, consistent with the high concentrations observed in the free
troposphere, implying that the air quality standard in South Korea is not
practically achievable unless this background external to East Asia can be
decreased.</p>
  </abstract>
    
<funding-group>
<award-group id="gs1">
<funding-source>Samsung Advanced Institute of Technology</funding-source>
<award-id>NA</award-id>
</award-group>
</funding-group>
</article-meta>
  </front>
<body>
      

<?pagebreak page4032?><sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e262">Surface ozone is a severe air quality problem in South Korea and has become
steadily worse over the past 2 decades (Gaudel et al., 2018; Yeo and Kim,
2021; Kim et al., 2021). Ozone often exceeds 90 ppb in the Seoul
metropolitan area (SMA), where 50 % of South Korea's population is located
(Miyazaki et al., 2019). In 2015, Phase 2 of the Seoul Metropolitan Air
Quality Control Master Plan established a national standard of 60 ppb for
the maximum daily 8 h average (MDA8) ozone concentration (MOE, 2016).
However, no monitoring sites have been compliant with this standard in
recent years, and ozone has continued to increase (NIER, 2020). Improved
understanding of the causes of elevated ozone in South Korea is crucial for
developing effective emission control strategies.</p>
      <p id="d1e265">Ozone is produced in the troposphere by photochemical oxidation of volatile
organic compounds (VOCs) in the
presence of nitrogen oxides (NO<inline-formula><mml:math id="M5" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> <inline-formula><mml:math id="M6" display="inline"><mml:mo>≡</mml:mo></mml:math></inline-formula> NO <inline-formula><mml:math id="M7" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> NO<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>). Both VOCs and NO<inline-formula><mml:math id="M9" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula>
have large anthropogenic sources from combustion, and VOCs also have
fugitive industrial and residential, as well as biogenic, sources.
Effectively reducing ozone concentrations requires knowledge of whether
ozone production is NO<inline-formula><mml:math id="M10" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> or VOC limited. In the
NO<inline-formula><mml:math id="M11" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula>-limited regime, decreasing NO<inline-formula><mml:math id="M12" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions decreases ozone, while
decreasing VOC emissions has little effect. In the VOC-limited regime, when
NO<inline-formula><mml:math id="M13" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> concentrations are very high, decreasing NO<inline-formula><mml:math id="M14" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions drives an
increase in
ozone, while decreasing VOC emissions decreases ozone (Sillman et al., 1990).
The Clean Air Policy Support System (CAPSS) bottom-up emission inventory in
South Korea reports emission declines of 26 % for NO<inline-formula><mml:math id="M15" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> and 25 % for VOCs
in Seoul over the 2000–2019 period
(<uri>https://www.air.go.kr/eng/capss/emission/sido.do?menuId=100</uri>, last access: 1 December 2022). Using
satellite and surface observations of 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>, Seo et al. (2021) found that NO<inline-formula><mml:math id="M17" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions declined in Seoul by 30 % during the 2015–2019 period, and Bae
et al. (2021) found an 18 % decrease for the 2015–2018 period. On the
other hand, Bauwens et al. (2022) found an increase in satellite-observed
HCHO columns over South Korea by 1 % a<inline-formula><mml:math id="M18" 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>–2 % a<inline-formula><mml:math id="M19" 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> for the 2005–2019 period,
which does not support a decrease in VOC emissions.</p>
      <p id="d1e410">Ozone concentrations over South Korea depend not only on domestic emissions
but also on the background from external sources. The KORUS-AQ (Korea–United States Air Quality) aircraft
campaign in May–June 2016 found free-tropospheric concentrations
above 2 km altitude frequently exceeding 80 ppb (Miyazaki et al., 2019;
Sullivan et al., 2019; Gaubert et al., 2020; Crawford et al., 2021), which
would affect surface ozone through subsidence. An obvious source of
background ozone is China, where ozone is very high and increasing (Li et
al., 2019, 2021) and would be transported to South Korea by westerly winds
(Cuesta et al., 2018). But other background sources could also contribute.
Lam and Cheung (2022) found that strong transport from the stratosphere can
enhance springtime surface ozone by up to 8 ppb in East Asia. Li et al. (2016) estimated from a global model that
long-range transport from outside East Asia could contribute 50 %–80 % to
annual surface ozone in the Korean Peninsula. Wang et al. (2022) found an
increase in free-tropospheric ozone over East Asia of 3.8 to 6.7 ppb per decade over the
1995–2017 period.</p>
      <p id="d1e413">The high and increasing ozone over South Korea could thus reflect a
combination of decreasing NO<inline-formula><mml:math id="M20" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions and/or increasing VOC emissions
under VOC-limited conditions for ozone production (Jung et al., 2018), as
well as high and increasing background ozone. Here we aim to better
understand the factors controlling ozone and its increase in the SMA and
more broadly over South Korea during the 2015–2019 period. We focus our
analysis on the 90th percentile MDA8 ozone as a robust metric for
polluted conditions (Fiore et al., 1998; Sun et al., 2017; Wells et al.,
2021). We use a random forest (RF) method (Grange et al., 2018) to correct
for the role of meteorology in driving the 2015–2019 ozone trend in the SMA
and show that meteorology-corrected ozone is highest in May–June and
increases the fastest in April–May, while showing no significant trend in
July–August.
We find that a 3-D chemical transport model driven by meteorological input from the Goddard Earth Observing System (GEOS-Chem) can successfully capture the magnitude and trends of ozone concentrations, including their seasonality. We use the model to quantify the importance of domestic and different background contributions in driving elevated ozone and its increase over South Korea.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>AirKorea data and trends, 2015–2019</title>
      <p id="d1e433">We use ozone and NO<inline-formula><mml:math id="M21" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations measured hourly by the AirKorea national
air quality network of the South Korea Ministry of Environment (<uri>http://www.airkorea.or.kr/web</uri>, last access: 3 October 2022). There are 255 sites in South Korea
covering the 2015–2019 period including 79 sites in the SMA defined here
as the rectilinear domain (37.2–37.8<inline-formula><mml:math id="M22" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 126.7–127.3<inline-formula><mml:math id="M23" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E). Figure 1 shows the maximum monthly
90th percentile MDA8 ozone at the ensemble of AirKorea sites for each
year from 2015 to 2019. Ozone rises steadily over that period except for a
dip in 2018, reaching 96 ppb in 2019 averaged across all AirKorea sites.
High values are spread throughout South Korea, and no site meets the 60 ppb
air quality standard. Also shown is the monthly time series of ozone for the
SMA. Ozone levels are similar to the rest of South Korea, though they do not show
the 2018 dip. The seasonal maximum is in May–August depending on the year.</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="d1e468">The 90th percentile maximum daily 8 h average (MDA8)
ozone concentrations in South Korea for 2015–2019. Panel <bold>(a)</bold> shows the
maximum monthly 90th percentile ozone at individual AirKorea sites. The
mean of this statistic across the ensemble of sites is shown inset. Panel <bold>(b)</bold> shows
90th percentile MDA8 ozone averaged for individual months over sites
within the Seoul metropolitan area (SMA; 37.2–37.8<inline-formula><mml:math id="M24" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 126.7–127.3<inline-formula><mml:math id="M25" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E), as well as for
all AirKorea sites. Tick marks are for June, and dashed lines are for
December. Only sites with over 90 % of observational coverage for the 2015–2019 period are included in this analysis.</p></caption>
        <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-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="d1e503">Same as Fig. 1 but for 24 h average annual mean 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>
concentrations.</p></caption>
        <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f02.png"/>

      </fig>

      <?pagebreak page4033?><p id="d1e522">Figure 2 shows the annual mean 24 h average NO<inline-formula><mml:math id="M27" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentration at the
ensemble of AirKorea sites. Concentrations 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> in the SMA are generally
10 ppb higher than averaged across South Korea. NO<inline-formula><mml:math id="M29" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations peak in
winter and are minimum in summer, as observed elsewhere in East Asia, and are
mostly driven by longer NO<inline-formula><mml:math id="M30" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> lifetime and reduced vertical mixing in winter
(Lamsal et al., 2010; Shah et al., 2020; Lin et al., 2019; Kim et al.,
2020). There is a decreasing trend over the 2015–2019 period as previously reported
by Seo et al. (2021), with this being the case more so in summer than in winter.</p>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Meteorological correction of 2015–2019 trends in the SMA</title>
      <p id="d1e569">The 2015–2019 trends in ozone and NO<inline-formula><mml:math id="M31" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations from Figs. 1 and 2
could reflect not only emission trends but also meteorological variability. Here we
use a random forest (RF) non-parametric statistical model (Breiman, 2001;
Tong et al., 2003) to isolate and remove the effect of meteorological variability
for the 79 AirKorea sites in the SMA (Fig. 3). RF is a supervised ensemble
machine learning method, where many individual uncorrelated decision trees
are fit to the
training data to predict an output value, with the average value taken as
the best estimate (Breiman, 2001). The RF model was
constructed using R “normalweatherr” packages (<uri>https://github.com/skgrange/normalweatherr</uri>, last access: 17 August 2022; Grange et al., 2018). Hourly
meteorological data are from two sites operated by the Korea Meteorological
Administration (KMA) within the SMA (<uri>https://data.kma.go.kr/data/grnd</uri>, last access: 21 June 2022). The RF model is trained to predict the
hourly ozone and NO<inline-formula><mml:math id="M32" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations averaged across the 79 AirKorea sites
using the meteorological data averaged for the two KMA sites as well as the time
of the day, the day of the year and a long-term linear trend (Unix timestamp).
Explanatory variables for the RF algorithm are listed in Table 1. Training of the RF model was conducted on 70 % of the input data, and
the other 30 %<?pagebreak page4034?> was withheld as testing data. The number of variables used
to grow a tree was set to 3, the minimum node size was 5 and the
number of trees within a forest was set to 300. Once trained, the RF model
is then used to predict ozone and NO<inline-formula><mml:math id="M33" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations based on randomly
sampled meteorological data, and predictions are aggregated as described
below.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e607">AirKorea monitoring sites in the Seoul metropolitan
area (SMA) with hourly ozone and NO<inline-formula><mml:math id="M34" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentration data for 2015–2019. Red
diamonds show the two meteorological sites in the SMA operated by the Korea
Meteorological Administration (<uri>https://data.kma.go.kr/data/grnd</uri>).</p></caption>
        <?xmltex \igopts{width=213.395669pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f03.png"/>

      </fig>

      <p id="d1e628">Figure 4 compares observed and predicted hourly concentrations of ozone and
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> for the data withheld from training. The RF model shows a strong
predictive ability (<inline-formula><mml:math id="M36" display="inline"><mml:mrow><mml:mi>R</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.93</mml:mn></mml:mrow></mml:math></inline-formula> for ozone, 0.90 for NO<inline-formula><mml:math id="M37" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>) with negligible mean
bias (0.23 ppb for ozone, 0.01 ppb for 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>) and a root mean square error
(RMSE) of 5.9 ppb for ozone and 6.2 ppb for 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>. The model has difficulty in
capturing the tails of the distribution, which is a well-recognized problem
in RF algorithms (Zhang and Lu, 2012; Pendergrass et al., 2022).</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1"><?xmltex \currentcnt{1}?><label>Table 1</label><caption><p id="d1e683">Random forest predictor variables
for hourly ozone and 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> concentrations<inline-formula><mml:math id="M41" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula>.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="1">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:thead>
       <oasis:row>
         <oasis:entry colname="col1">Meteorology<inline-formula><mml:math id="M51" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><?xmltex \hack{\hspace*{0.5cm}}?>Wind speed</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><?xmltex \hack{\hspace*{0.5cm}}?>Wind direction</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><?xmltex \hack{\hspace*{0.5cm}}?>Temperature</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><?xmltex \hack{\hspace*{0.5cm}}?>Surface pressure</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"><?xmltex \hack{\hspace*{0.5cm}}?>Relative humidity</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Time</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><?xmltex \hack{\hspace*{0.5cm}}?>Day of the year<inline-formula><mml:math id="M52" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">c</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><?xmltex \hack{\hspace*{0.5cm}}?>Unix time<inline-formula><mml:math id="M53" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">d</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><?xmltex \hack{\hspace*{0.5cm}}?>Hour of the day</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><table-wrap-foot><p id="d1e704"><inline-formula><mml:math id="M42" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula> Hourly explanatory variables in the random forest (RF) model fitted
to hourly ozone and 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> concentrations averaged across 79 AirKorea sites in
the Seoul metropolitan area (SMA) for 2015–2019.
<inline-formula><mml:math id="M44" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula> Meteorological data are from the two SMA stations for synoptic meteorological observation (<uri>https://data.kma.go.kr/data/grnd</uri>) located at Gwanaksan (37.345<inline-formula><mml:math id="M45" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 126.975<inline-formula><mml:math id="M46" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) and in Seoul (37.585<inline-formula><mml:math id="M47" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 126.980<inline-formula><mml:math id="M48" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E).
Data are averaged across the two stations for input to the RF model.
<inline-formula><mml:math id="M49" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">c</mml:mi></mml:msup></mml:math></inline-formula> Day of the year, used as a seasonal term.
<inline-formula><mml:math id="M50" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">d</mml:mi></mml:msup></mml:math></inline-formula> Used as a linear-trend term.</p></table-wrap-foot><?xmltex \gdef\@currentlabel{1}?></table-wrap>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e899">Performance of the random forest (RF) model in fitting
2015–2019 hourly ozone and NO<inline-formula><mml:math id="M54" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations in the Seoul metropolitan area
(SMA). The RF model is trained on hourly concentrations averaged across 79
AirKorea monitoring sites in the SMA (Fig. 3). The figure compares
predicted and observed values for the 30 % of data withheld from training.
Comparison statistics are shown inset including the root mean square error
(RMSE), correlation coefficient (<inline-formula><mml:math id="M55" display="inline"><mml:mi>R</mml:mi></mml:math></inline-formula>) and mean bias (MB). Also shown are the
1 : 1 lines. Count refers to the number of data points within a given (ozone,
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>) data bin (individual symbol).</p></caption>
        <?xmltex \igopts{width=312.980315pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f04.png"/>

      </fig>

      <p id="d1e933">The top predictors in the RF fit for ozone are the temperature, day of the year,
relative humidity, hour of the day and wind speed, in that order, consistent
with previous studies for urban areas (Sillman and Samson, 1995; Jacob and
Winner, 2009; Li et al., 2020). The top predictors for NO<inline-formula><mml:math id="M57" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> are the wind
speed, day of the year, temperature, hour of the day and surface pressure, again
consistent with previous studies (Liu et al., 2020; Richmond-Bryant et al.,
2018).</p>
      <p id="d1e945">We use the RF model to remove the effect of meteorological variability in
driving the 2015–2019 ozone 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> trends by following the technique
outlined in Vu et al. (2019). Meteorological variables for a specific hour
and date in the input dataset are replaced by randomly selecting weather
data over the entire study period (2015–2019) at that hour of the day but for
a different day of the year within a 4-week period (2 weeks before to 2 weeks
after the selected date). This process is repeated 1000 times, and the
resulting 1000 RF predictions of ozone and NO<inline-formula><mml:math id="M59" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> for that hour and date are
then averaged to produce meteorology-corrected concentrations from which we
recalculate MDA8 ozone and 24 h averaged 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> to infer 2015–2019
emission-driven trends.</p>
</sec>
<sec id="Ch1.S4">
  <label>4</label><?xmltex \opttitle{Emission-driven trends in ozone and NO${}_{2}$ concentrations in the SMA, 2015--2019}?><title>Emission-driven trends in ozone and NO<inline-formula><mml:math id="M61" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations in the SMA, 2015–2019</title>
      <?pagebreak page4035?><p id="d1e993">Figure 5 shows the observed and meteorology-corrected trends of monthly
90th percentile MDA8 ozone concentrations in the SMA from 2015 to 2019.
The observations show peak increase in May but a highly variable trend from
month to month driven in part by interannual meteorological variability. The
meteorology-corrected data show a much smoother behavior with a broad
springtime (March–May) maximum in the increasing ozone trend and a
decreasing trend in August. Meteorology-corrected ozone is highest in
May–June for all years. The 2015–2019
trend in meteorology-corrected 90th percentile ozone is 0.7, 1.4 and
0.4 ppb a<inline-formula><mml:math id="M62" 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> for winter, spring and fall. The overall trend for
summer is not statistically significant, but the trend for June alone is 0.9 ppb a<inline-formula><mml:math id="M63" 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>. This seasonality of ozone trends in the SMA from 2015 to 2019
is consistent with the 2000–2014 results of Jung et al. (2018), who reported
a maximum springtime ozone increase in South Korea and an advancement of the
ozone season by 2.1 d a<inline-formula><mml:math id="M64" 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>. Similar seasonality in the ozone trend
has been reported for the North China Plain (Li et al., 2021), showing a
2-fold increase in May ozone exceedances above the 75 ppb standard from
2014 to 2019. Ozone production is most likely to be NO<inline-formula><mml:math id="M65" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> limited in summer
when solar radiation and biogenic emissions are highest and VOC limited in
spring and fall (Jacob et al., 1995); thus the seasonality of the trend is
consistent with VOC-limited conditions.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><?xmltex \currentcnt{5}?><?xmltex \def\figurename{Figure}?><label>Figure 5</label><caption><p id="d1e1043">The 2015–2019 trends in monthly 90th percentile MDA8
ozone averaged across the 79 AirKorea sites in the Seoul metropolitan area
(SMA). Panels <bold>(a)</bold> and <bold>(c)</bold> show the observed trends for individual months, and
panels <bold>(b)</bold> and <bold>(d)</bold> show meteorology-corrected trends. Panels <bold>(c)</bold> and <bold>(d)</bold> show
the 2015–2019 slopes for individual months obtained by ordinary least-squares
regressions of the data in panels <bold>(a)</bold> and <bold>(b)</bold>.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f05.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6"><?xmltex \currentcnt{6}?><?xmltex \def\figurename{Figure}?><label>Figure 6</label><caption><p id="d1e1080">Same as Fig. 5 but for 24 h average NO<inline-formula><mml:math id="M66" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations.
Trends are shown in percent per annum relative to the 2015–2019 mean.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f06.png"/>

      </fig>

      <?pagebreak page4036?><p id="d1e1098">Figure 6 is the same as Fig. 5 but for 24 h average NO<inline-formula><mml:math id="M67" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations. The
observations show a <inline-formula><mml:math id="M68" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> % a<inline-formula><mml:math id="M69" 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> decrease in all months
except November–February. The meteorology-corrected data show a consistent
5.6 % a<inline-formula><mml:math id="M70" 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> decrease in March–October, or 22 % over the 4 years,
and a consistent but weaker 1.5 % a<inline-formula><mml:math id="M71" 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> decrease in November–February.
This is consistent with findings from Bae et al. (2021), who reported a
4.4 % a<inline-formula><mml:math id="M72" 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> decline in annual mean 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> in the SMA for 2015–2018 using
surface and satellite observations. Declining 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> in the SMA can be
attributed to policies to decrease vehicular NO<inline-formula><mml:math id="M75" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions (Kim and Lee,
2018). The weaker decline in winter is consistent with findings from Seo et
al. (2021), who found that surface 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> concentrations in the SMA in
2015–2019 declined by 5.3 % a<inline-formula><mml:math id="M77" 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> during the time of the morning commute for the
ozone season but only by 2.6 % a<inline-formula><mml:math id="M78" 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> for the non-ozone season. The
weaker response of 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> to reduced NO<inline-formula><mml:math id="M80" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions in winter could be due to
ozone titration by emitted NO, which would take place most systematically at
night but also extend to daytime if the ozone supply is weak. We find that
in November–February the decline in NO<inline-formula><mml:math id="M81" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> during midday (11:00–15:00 LT) is
2.4 % a<inline-formula><mml:math id="M82" 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>, greater than twice that at night (23:00–03:00 LT),
consistent with ozone titration. For the GEOS-Chem simulations in the
following sections we will assume a 22 % decrease in NO<inline-formula><mml:math id="M83" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions from
2015 to 2019.</p>
</sec>
<sec id="Ch1.S5">
  <label>5</label><title>GEOS-Chem simulation</title>
      <p id="d1e1287">We use the GEOS-Chem chemical transport model version 13.3.4 (<uri>http://geos-chem.org</uri>, last access: 27 October 2022) to interpret the observed ozone and its 2015–2019
trend in the SMA and more broadly in South Korea, including influences from
China and the global background. GEOS-Chem has been applied previously in
South Korea to investigate ozone production efficiency (Oak et al., 2019),
the factors determining ozone seasonality (Lee and Park, 2022) and the
photochemical environment for ozone production (Yang et al., 2023). Park et
al. (2021) previously found that GEOS-Chem version 12.7.2 underestimated free-tropospheric ozone over South Korea by 20–30 ppb.
Addition of detailed aromatic chemistry in version 13.3.4 (Bates et al.,
2021) was subsequently found to increase net ozone production over South
Korea by 37 % (Oak et al., 2019). Here we also add particulate nitrate
photolysis and suppression of sea salt aerosol debromination to the model
following Shah et al. (2023), and as we will see this largely corrects the
remaining model ozone bias over East Asia.</p>
      <p id="d1e1293">We use a nested-grid version of GEOS-Chem driven by MERRA-2-assimilated (Modern-Era Retrospective analysis for Research and Applications)
meteorological data with a horizontal resolution of 0.5<inline-formula><mml:math id="M84" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M85" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.625<inline-formula><mml:math id="M86" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>
over East Asia (25–50<inline-formula><mml:math id="M87" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 105–140<inline-formula><mml:math id="M88" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E; domain
of Fig. 7). Chemical boundary conditions at the edges of the nested domain
are updated every 3 h from a global simulation with 4<inline-formula><mml:math id="M89" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M90" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 5<inline-formula><mml:math id="M91" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>
resolution. We conduct a full-year simulation for 2016 with 6 months of
initialization. Global anthropogenic emissions are from the Community
Emissions Data System (CEDS) global inventory (Hoesly et al., 2018) and are
superseded with regional emission inventories for South Korea (KORUSv5,
<uri>http://aisl.konkuk.ac.kr</uri>, last access: 13 May 2022) and China (Multi-resolution Emission Inventory model for Climate and air pollution research, MEIC;
Zheng et al., 2018). Natural emissions include NO<inline-formula><mml:math id="M92" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> from lightning (Murray et
al., 2012) and soil (Hudman et al., 2012), MEGANv2 biogenic volatile organic
compounds (VOCs) (Guenther et al., 2012), dust (Meng et al., 2021), and sea
salt (Jaeglé et al., 2011). Open-fire emissions are from the Global Fire
Emissions Database version 4 (GFED4; van der Werf et al., 2017).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7"><?xmltex \currentcnt{7}?><?xmltex \def\figurename{Figure}?><label>Figure 7</label><caption><p id="d1e1379">Monthly 90th percentile MDA8 ozone over South Korea
and China for different seasons in 2016. GEOS-Chem model results for each
season (background contours) are compared to AirKorea and MEE network
observations (symbols); 50 % of network sites have been culled randomly
for visualization purposes. The GEOS-Chem correlation coefficient (<inline-formula><mml:math id="M93" display="inline"><mml:mi>R</mml:mi></mml:math></inline-formula>) and mean
bias (MB) relative to observations are shown inset. DJF: December–January–February, MAM: March–April–May, JJA: June–July–August, SON: September–October–November.</p></caption>
        <?xmltex \igopts{width=199.169291pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f07.png"/>

      </fig>

      <p id="d1e1396">Ships are a relatively large source of NO<inline-formula><mml:math id="M94" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> in East Asia. The standard
GEOS-Chem model includes pre-processing of ship emissions with the
PARAmeterization of emitted NO<inline-formula><mml:math id="M95" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> (PARANOX) algorithm (Vinken et al., 2011) to
account for the non-linear chemistry occurring during the dispersion of ship
exhaust plumes. PARANOX is a plume-in-grid formulation where ship emissions
are aged chemically for 5 h before being released into the model grid.
This greatly reduces the ozone yield from ship NO<inline-formula><mml:math id="M96" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions, which would
otherwise be diluted by the model in a relatively clean environment where
the ozone production efficiency is very high. PARANOX was intended for
global model simulations with a grid resolution of hundreds of kilometers (Holmes et
al., 2014), and its application to higher-resolution simulations is
questionable, particularly over East Asia, where the maritime environment is
highly polluted (Cuesta et al., 2018; Peterson et al., 2019; Jung et al.,
2022). Here we disable PARANOX for the nested simulation and find that this
increases ozone over the Yellow Sea in May by 1 ppb on average.</p>
      <p id="d1e1426">We evaluate our GEOS-Chem simulation for 2016 with MDA8 ozone observations
from the AirKorea network in South Korea and the Ministry of Ecology and
Environment (MEE) monitoring network in China
(<uri>http://data.epmap.org/page/index</uri>, last access: 9 July 2022). Observations of seasonal mean 90th
percentile MDA8 ozone overlaid on our GEOS-Chem simulation are shown in
Fig. 7. There is good agreement between GEOS-Chem and observations in all
seasons, with a spatial correlation coefficient <inline-formula><mml:math id="M97" display="inline"><mml:mrow><mml:mi>R</mml:mi><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">0.7</mml:mn></mml:mrow></mml:math></inline-formula> and a mean
bias <inline-formula><mml:math id="M98" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:math></inline-formula> ppb.</p>
      <?pagebreak page4037?><p id="d1e1454"><?xmltex \hack{\newpage}?>We evaluated GEOS-Chem's ability to reproduce the seasonal cycle of ozone in
the three megacity clusters of the Seoul metropolitan area (SMA),
Beijing–Tianjin–Hebei (BTH) and the Yangtze River Delta (YRD). Figure 8 shows
the monthly 90th percentile MDA8 ozone for 2016 averaged over all
network sites in each cluster. The simulated seasonal cycle is consistent
with observations (<inline-formula><mml:math id="M99" display="inline"><mml:mrow><mml:mi>R</mml:mi><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">0.95</mml:mn></mml:mrow></mml:math></inline-formula> and mean bias <inline-formula><mml:math id="M100" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">6.0</mml:mn></mml:mrow></mml:math></inline-formula> ppb).</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="d1e1482">Seasonal variation in monthly 90th percentile MDA8
ozone in three megacity clusters in 2016. The clusters are the Seoul
metropolitan area (SMA; 37.2–37.8<inline-formula><mml:math id="M101" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 126.7–127.3<inline-formula><mml:math id="M102" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E), the Yangtze River Delta (YRD;
30–33<inline-formula><mml:math id="M103" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 118–122<inline-formula><mml:math id="M104" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) and
Beijing–Tianjin–Hebei (BTH; 37–41<inline-formula><mml:math id="M105" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 114–118<inline-formula><mml:math id="M106" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E). GEOS-Chem results are compared to observations, and the
corresponding root mean square error (RMSE) and mean bias (MB) are shown
inset. The 90th percentiles are computed from the time series of
spatial mean concentrations for each cluster, with GEOS-Chem sampled at the
network sites.</p></caption>
        <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f08.png"/>

      </fig>

      <p id="d1e1546">May is of particular interest in the SMA because this is when ozone and its
increasing trend are highest in the meteorology-corrected data (Fig. 5).
Previous model comparisons to extensive vertical profiles taken during the
KORUS-AQ aircraft campaign over South Korea in May–June 2016 showed large
underestimates, with GEOS-Chem version 12.7.2 being too low by 20–30 ppb
(Park et al., 2021). The model updates described above largely
correct this underestimate (Yang et al., 2023). Figure 9 compares our
simulated GEOS-Chem ozone profile to the mean of 15 ozonesonde observations
over Olympic Park in Seoul taken during the KORUS-AQ campaign on DC-8 flight
observation days (15 profiles in total). Our simulation has a low bias of
only 5.4 ppb in the free troposphere.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9" specific-use="star"><?xmltex \currentcnt{9}?><?xmltex \def\figurename{Figure}?><label>Figure 9</label><caption><p id="d1e1552">Mean vertical ozone profile over Olympic Park
(37.522<inline-formula><mml:math id="M107" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 127.124<inline-formula><mml:math id="M108" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) and Taehwa Research Forest
(37.312<inline-formula><mml:math id="M109" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 127.310<inline-formula><mml:math id="M110" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E) in Seoul during KORUS-AQ (May–June 2016). Observations from Olympic Park and Taehwa are from 15 and 42 ozonesondes, respectively. Ozonesondes were launched between 13:00 and 14:00 local time on KORUS-AQ flight days. GEOS-Chem model results are sampled at
the observation times. The circles show the surface ozone concentrations
from GEOS-Chem and the AirKorea site in the closest proximity.</p></caption>
        <?xmltex \igopts{width=312.980315pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f09.png"/>

      </fig>

      <p id="d1e1597">To investigate and diagnose the ability of GEOS-Chem to reproduce the
observed 2015–2019 ozone trend in the SMA, we performed simulations with
2016 meteorology (January–December 2016) and perturbed emissions in
China and South Korea for 2015 and 2019 to simulate the 2015–2019 trend. The
sensitivity simulations used 6 months of initialization. China emissions in
2015 are from MEIC (Zheng et al., 2018), but MEIC does not extend beyond
2017. Following Li et al. (2021), we scaled 2017 MEIC emissions to 2019
based on observed MEE network trends. Overall, emissions in China declined
from 2015 to 2019 by 16 % for NO<inline-formula><mml:math id="M111" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula>, 50 % for SO<inline-formula><mml:math id="M112" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, 23 % for CO and
32 % for primary PM<inline-formula><mml:math id="M113" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula>, with flat VOC emissions (Li et al., 2021).
Anthropogenic emissions for South Korea in 2015 are taken from the KORUSv5
inventory (<uri>http://aisl.konkuk.ac.kr</uri>). For 2019 we decrease NO<inline-formula><mml:math id="M114" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions in
South Korea by 22 % (Sect. 4) and apply no other changes to South Korea
emissions, including VOCs for which emission trends are not clear, as
mentioned in the Introduction. We also do not apply trends to ship
emissions.</p>

      <?xmltex \floatpos{p}?><fig id="Ch1.F10"><?xmltex \currentcnt{10}?><?xmltex \def\figurename{Figure}?><label>Figure 10</label><caption><p id="d1e1641">Emission-driven trends in 90th percentile MDA8
ozone from 2015 to 2019 in the Seoul metropolitan area (SMA) for individual
months. The observed meteorology-corrected trend is as shown in Fig. 5.
The modeled trend is obtained by subtraction of results from simulations
with 2015 and 2019 emissions, both using the same 2016 meteorology.</p></caption>
        <?xmltex \igopts{width=184.942913pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f10.png"/>

      </fig>

      <p id="d1e1650">Figure 10 shows the emission-driven trends of 90th percentile MDA8
ozone from 2015 to 2019 in the SMA for both meteorology-corrected
observations (data from Fig. 5) and GEOS-Chem in individual months. The
model trend is obtained by the subtraction of results from simulations with 2015
and 2019 emissions, both using the same 2016 meteorology. GEOS-Chem
reproduces the general magnitude and seasonality of the observed trend. It
reproduces in particular the April–May maximum in the trend.</p>
</sec>
<sec id="Ch1.S6">
  <label>6</label><title>Attribution of ozone and its 2015–2019 trend over South Korea</title>
      <p id="d1e1661">We exploit the success of GEOS-Chem in simulating ozone over East Asia and
its trend over the SMA to investigate the causes. We focus on May, where
both ozone concentrations and the increasing trend in the meteorology-corrected data for the SMA are the highest. In addition to the baseline
simulation described in Sect. 5, we also conduct sensitivity simulations
for both emission years to isolate the effects of anthropogenic emissions
from South Korea, China, ships and East Asia as a whole by zeroing the
corresponding emissions including NO<inline-formula><mml:math id="M115" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula>, VOCs, CO and PM<inline-formula><mml:math id="M116" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula>. The same global
boundary conditions described above are used for each of these cases, with 6 months of initialization.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F11"><?xmltex \currentcnt{11}?><?xmltex \def\figurename{Figure}?><label>Figure 11</label><caption><p id="d1e1684">Emission-driven ozone changes over East Asia from 2015
to 2019 in GEOS-Chem. Results show the 90th percentile MDA8 ozone for
May simulated by GEOS-Chem using 2015 emissions, as well as the difference using
2019 emissions, both for the same meteorological year. Panels <bold>(a)</bold> and <bold>(b)</bold> show the
baseline simulation described and evaluated with observations in Sect. 5.
Panels <bold>(c)</bold>–<bold>(f)</bold> show sensitivity simulations with zero
anthropogenic emissions in South Korea and China, respectively. Spatially
averaged values for the Seoul metropolitan area (SMA) and South Korea are
given inset.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f11.png"/>

      </fig>

      <p id="d1e1705">Figure 11 shows the distribution of simulated 90th percentile MDA8
ozone for May using 2015 emissions, the difference when using 2019
emissions, and the contributions from South Korea and China as determined
from the sensitivity simulations with the corresponding emissions shut off.
The 2015 values in the baseline simulation average
85.8 ppb in the SMA and 90.1 ppb for all of South Korea, and the 2019–2015
difference averages <inline-formula><mml:math id="M117" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula>6.2 ppb for the SMA, while southern parts of the
country show decreases. Zeroing out South Korea emissions has remarkably
little
effect on SMA concentrations, which remain at 84.1 ppb for 2015, though the
2015–2019 trend is now near zero. Zeroing out China emissions decreases SMA
ozone concentrations to 79.8 ppb, but the 2015–2019 increase remains at 5.6 ppb. We conclude that the 2015–2019 ozone increase in the SMA can be
attributed to the decrease in domestic NO<inline-formula><mml:math id="M118" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions under VOC-limited
conditions. When emissions from China are zeroed out, we find a 6 ppb ozone
decrease in the SMA and an 8 ppb decrease in South Korea as a whole compared
to the baseline simulation. The 2015–2019 ozone trend over the SMA is
affected by less than 1 ppb, confirming that this trend is mainly driven by
domestic emission changes.</p>
      <p id="d1e1725">A notable result is that ozone levels over South Korea remain very high at
about 80 ppb even when emissions from either South Korea or China are
totally shut off. Lee and Park (2022) previously found with GEOS-Chem that
surface ozone over South Korea in April hardly changes when domestic
emissions are shut off, and here we find that zeroing China emissions also
has only a modest effect over South Korea. This resilience is indicative of
a major contribution to ozone pollution from the northern midlatitude
background external to East Asia.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F12" specific-use="star"><?xmltex \currentcnt{12}?><?xmltex \def\figurename{Figure}?><label>Figure 12</label><caption><p id="d1e1730">East Asia background ozone and individual enhancements
due to anthropogenic emissions from ships in the Yellow Sea (north of
30.5<inline-formula><mml:math id="M119" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), South Korea and China. Results show the monthly mean
90th percentile MDA8 ozone for May simulated by GEOS-Chem for
meteorological year 2016.</p></caption>
        <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/4031/2023/acp-23-4031-2023-f12.png"/>

      </fig>

      <p id="d1e1748">Figure 12 further explores the role of this East Asia background in a
simulation with anthropogenic emissions shut off throughout the nested model
domain. The 90th percentile MDA8 ozone drops to 55 ppb in South Korea,
meeting the 60 ppb standard but still extremely high and indicating that
even low anthropogenic emissions would cause ozone to rise above the
standard. This high East Asia background affects northern China even more.
Lam and Cheung (2022) previously found with GEOS-Chem that the mean MDA8
background ozone over China in April is 53 ppb, and we find here that the
90th percentile over northern China reaches 70 ppb. This East Asia
background ozone is much higher than the corresponding North America
background of 20–40 ppb previously reported in studies of US ozone pollution
(Fiore et al., 2003; Zhang et al., 2011; Emery et al., 2012; Jaffe et al.,
2018). Such a high East Asia background is reflected in the observation of
75 ppb ozone in the free troposphere (Fig. 9), while comparable ozonesonde
observations over the western US in spring show mean values of 60 ppb (Zhang
et al., 2011). Satellite observations of free-tropospheric ozone also show
particularly high values over East Asia (Hu et al., 2017; Gaudel et al.,
2018). High free-tropospheric ozone over East Asia in spring could reflect
regional downwelling from the stratosphere associated with cyclogenesis
(Hwang et al., 2007). It could also reflect the observed rise in free-tropospheric ozone at northern midlatitudes and particularly over East Asia
in recent decades (Gaudel et al., 2018; Lee et al., 2021; Wang et al., 2022),
which could possibly be due to increasing emissions in India and the Middle
East (Anwar et al., 2021; Ding et al., 2022; Anenberg et al., 2022). We find
from analysis of sonde observations at Pohang, South Korea;<?pagebreak page4039?> Hong Kong SAR, China; and Tateno, Japan
(<uri>https://woudc.org/data/dataset_info.php?id=ozonesonde</uri>, last access: 5 August 2022), no
significant trend in free-tropospheric ozone over South Korea during
2015–2019, meaning that the background is not responsible for the observed
increase in surface ozone over that period. Domestic emissions are likely
responsible, as discussed above.</p>
      <p id="d1e1754">Additional panels in Fig. 12 show the enhancement of ozone above the East
Asia background due to emissions from the Yellow Sea (ships), South Korea
and China. Emissions from ships in the Yellow Sea enhance 90th
percentile MDA8 ozone over South Korea by only a few parts per billion, although they can
drive ozone concentrations over the
ocean in excess of 90 ppb. Despite ship traffic in the Yellow Sea being
intense, the NO<inline-formula><mml:math id="M120" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions are still low relative to continental
emissions. Emissions from South Korea alone push ozone to almost 80 ppb over
South Korea, with even larger increases over the surrounding oceans
reflecting VOC-limited conditions over land. In this way, emissions in South
Korea push ozone in the Shandong Peninsula in China to over 80 ppb.
Emissions in China have an effect on ozone over South Korea comparable to
domestic emissions.</p>
</sec>
<sec id="Ch1.S7" sec-type="conclusions">
  <label>7</label><title>Conclusions</title>
      <p id="d1e1774">We examined the factors controlling the high and increasing surface ozone
concentrations over South Korea and particularly in the Seoul metropolitan
area (SMA). Ozone in South Korea has risen steadily over the past 2 decades and is everywhere far in excess of the 60 ppb air quality standard
set by the government of South Korea in 2015. Improved understanding of the
causes of elevated ozone in South Korea is critical for developing effective
emission control strategies.</p>
      <p id="d1e1777">We find a continuation of the multidecadal increase in surface ozone in
South Korea. Analysis of 2015–2019 data from the AirKorea network of air
quality monitoring sites shows elevated ozone throughout South Korea, with
90th percentile ozone averaged across all sites exceeding 75 ppb every
year and increasing over the period. NO<inline-formula><mml:math id="M121" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations also measured at
AirKorea sites are typically <inline-formula><mml:math id="M122" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">10</mml:mn></mml:mrow></mml:math></inline-formula> ppb higher in the
SMA than elsewhere, with maximum concentrations in winter and a decrease
over the 2015–2019 period.</p>
      <p id="d1e1799">We used a random forest (RF) non-parametric statistical model to isolate and
remove the effect of meteorological variability on 2015–2019 ozone and NO<inline-formula><mml:math id="M123" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>
trends in the SMA. Meteorology-corrected ozone is highest in May–June for
all years and increases at the fastest rate of 1.5 ppb a<inline-formula><mml:math id="M124" 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> in
April–May. Meteorology-corrected NO<inline-formula><mml:math id="M125" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> is highest during November–March and
lowest in July–August. During the ozone season of March–October, NO<inline-formula><mml:math id="M126" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> shows a
consistent decline of 5.6 % a<inline-formula><mml:math id="M127" 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> over the 2015–2019 period, whereas in
winter the decline is lower at 1.3 % a<inline-formula><mml:math id="M128" 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>. The March–October trend in
NO<inline-formula><mml:math id="M129" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations suggests that NO<inline-formula><mml:math id="M130" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions declined by 22 % from 2015
to 2019.</p>
      <p id="d1e1884">We used the GEOS-Chem chemical transport model to interpret the elevated
ozone and its 2015–2019 trend in SMA and more broadly in South Korea,
including influences from China and the global background. We improved on
previous versions of the model, which substantially underestimated
tropospheric ozone over South Korea, through the addition of detailed
aromatic chemistry in version 13.3.4 (Bates et al., 2021), the removal of
sea salt aerosol debromination and the addition of particulate nitrate
photolysis (Shah et al., 2023). The resulting model can reproduce the
seasonality and spatial distribution of surface ozone in South Korea and
China without significant bias. It reproduces the high free-tropospheric
ozone concentrations observed over Seoul during the KORUS-AQ campaign in
May–June 2016 (75 <inline-formula><mml:math id="M131" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 7 ppb) with a bias that is only 5 ppb too low. Implementing in
the model the 2015–2019 emission decreases in South Korea and China reproduces the
observed seasonality and magnitude of the meteorology-corrected ozone trend
over the SMA.</p>
      <?pagebreak page4040?><p id="d1e1895"><?xmltex \hack{\newpage}?>We used GEOS-Chem sensitivity simulations for emission years 2015 and 2019
to better understand the factors contributing to elevated ozone in the SMA
and South Korea, focusing on May, when meteorology-corrected ozone and its
increase are the highest. We find that the 2015–2019 ozone increase in the
SMA can be explained by the 22 % decrease in surface NO<inline-formula><mml:math id="M132" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations,
which act as a proxy for declining NO<inline-formula><mml:math id="M133" display="inline"><mml:msub><mml:mi/><mml:mi>x</mml:mi></mml:msub></mml:math></inline-formula> emissions, reflecting the VOC-limited conditions for ozone production. We also find that emissions in
China and South Korea contribute equally to elevated ozone over South Korea,
while ships only contribute a small amount. VOC emission reductions would be
expected to decrease ozone in South Korea, but we find that concentrations
remain over 80 ppb even if all anthropogenic emissions from South Korea or
from China are zeroed out. The East Asia background, defined by zeroing out
all anthropogenic emissions over East Asia, is very high at 55 ppb, implying
that the 60 ppb air quality standard in South Korea is not achievable
without addressing the origin of this elevated background.</p>
</sec>

      
      </body>
    <back><notes notes-type="codeavailability"><title>Code availability</title>

      <p id="d1e1921">The code used in this work is available upon request.</p>
  </notes><notes notes-type="dataavailability"><title>Data availability</title>

      <p id="d1e1927">Ground-based measurements from the AirKorea national air quality network of
the South Korea Ministry of Environment are available at <uri>http://www.airkorea.or.kr/web</uri> (South Korea Ministry of Environment, 2022). Ozonesonde data from the KORUS-AQ data
archive are available at <uri>https://www-air.larc.nasa.gov</uri>
(Crawford et al., 2021). Meteorological data from the Korea
Meteorological Administration (KMA) are found at <uri>https://data.kma.go.kr/data/grnd</uri> (Korea
Meteorological Administration, 2022).</p>
  </notes><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e1942">The original draft preparation was done by NKC, with review and editing by DJJ, LHY, SZ, VS, SKG, RMY, SK and HL.
DJJ contributed to the project conceptualization.
Modeling was done by NKC, with additional support from LHY, SZ, VS and RMY.
The formal analysis was conducted by NKC with additional support from DJJ, LHY, SZ, VS, SKG and SK.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e1948">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="d1e1954">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="d1e1961">We
thank Zongbo Shi and Tuan Vu for their helpful insight into removing the
effect of meteorology on pollutant trends.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e1966">This work was funded by the Samsung Advanced Institute of Technology and the
Harvard–Nanjing University of Information Science &amp; Technology (NUIST) Joint Laboratory for Air Quality and Climate (JLAQC).</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e1972">This paper was edited by Bryan N. Duncan and reviewed by two anonymous referees.</p>
  </notes><ref-list>
    <title>References</title>

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