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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-25-14865-2025</article-id><title-group><article-title>Widespread stratospheric intrusion influence on summer ozone pollution over China revealed by multi-site ozonesonde and validated EAC4 reanalysis</article-title><alt-title>Stratospheric ozone intrusion in China</alt-title>
      </title-group>
      <contrib-group>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Liao</surname><given-names>Zhiheng</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Zhang</surname><given-names>Jinqiang</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Gao</surname><given-names>Meng</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-8657-3541</ext-link></contrib>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Ma</surname><given-names>Zhiqiang</given-names></name>
          <email>zqma@ium.cn</email>
        </contrib>
        <aff id="aff1"><label>1</label><institution>Institute of Urban Meteorology, China Meteorological Administration, Beijing, China</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>State Key Laboratory of Atmospheric Environment and Extreme Meteorology, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, China</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Department of Geography, Hong Kong Baptist University, Hong Kong SAR, China</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Zhiqiang Ma (zqma@ium.cn)</corresp></author-notes><pub-date><day>5</day><month>November</month><year>2025</year></pub-date>
      
      <volume>25</volume>
      <issue>21</issue>
      <fpage>14865</fpage><lpage>14877</lpage>
      <history>
        <date date-type="received"><day>2</day><month>January</month><year>2025</year></date>
           <date date-type="rev-request"><day>31</day><month>March</month><year>2025</year></date>
           <date date-type="rev-recd"><day>16</day><month>June</month><year>2025</year></date>
           <date date-type="accepted"><day>14</day><month>August</month><year>2025</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2025 Zhiheng Liao et al.</copyright-statement>
        <copyright-year>2025</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/25/14865/2025/acp-25-14865-2025.html">This article is available from https://acp.copernicus.org/articles/25/14865/2025/acp-25-14865-2025.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/25/14865/2025/acp-25-14865-2025.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/25/14865/2025/acp-25-14865-2025.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d2e122">Understanding stratospheric intrusion (SI) is crucial for elucidating atmospheric complexities and improving strategies to mitigate surface ozone (O<sub>3</sub>) pollution. This study investigates a deep trough-induced SI event in China from 10 to 13 June 2013, based on ozonesondes from Beijing, Changchun, and Hong Kong, and validated O<sub>3</sub> reanalysis products. Ozonesondes from Beijing indicated notable upper-level secondary O<sub>3</sub> peaks (<inline-formula><mml:math id="M4" display="inline"><mml:mo lspace="0mm">&gt;</mml:mo></mml:math></inline-formula> 400 ppbv) since 11 June. Tropospheric sub-high O<sub>3</sub> layers were observed in Changchun on 12 June (<inline-formula><mml:math id="M6" display="inline"><mml:mo lspace="0mm">&gt;</mml:mo></mml:math></inline-formula> 120 ppbv) and Hong Kong on 13 June (<inline-formula><mml:math id="M7" display="inline"><mml:mo lspace="0mm">&gt;</mml:mo></mml:math></inline-formula> 80 ppbv). Nationwide surface measurements recorded severe O<sub>3</sub> pollution (<inline-formula><mml:math id="M9" display="inline"><mml:mo lspace="0mm">&gt;</mml:mo></mml:math></inline-formula> 100 ppbv) from western plateaus to eastern plains over China. Together, these observations suggest a widespread influence of stratospheric O<sub>3</sub> intrusion. Further, the ozonesonde-validated EAC4 reanalysis reproduced the fine-scale SI structure (O<sub>3</sub>-rich “tongue”), in turn well explaining the secondary O<sub>3</sub> peaks and sub-high O<sub>3</sub> layers in ozonesonde observations. The O<sub>3</sub>-rich “tongue” swept through the Tibetan Plateau on 10 June, triggering extreme O<sub>3</sub> pollution with a stratospheric contribution up to 30 ppbv (<inline-formula><mml:math id="M16" display="inline"><mml:mo lspace="0mm">&gt;</mml:mo></mml:math></inline-formula> 30 %). With the trough's eastward movement, the O<sub>3</sub>-rich “tongue” penetrated into the lower troposphere of eastern China, and then entrained into the surface layer, exacerbating surface O<sub>3</sub> pollution occurred in eastern China on 13 June, with a stratospheric O<sub>3</sub> contribution of 3–15 ppbv (2 %–10 %). This research underscores the importance of multi-site ozonesondes in understanding stratospheric O<sub>3</sub> intrusions and the potential of the publicly available EAC4 reanalysis in multiyear SI analyses.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d2e307">Surface ozone (O<sub>3</sub>) poses significant risks to public health and ecosystem productivity due to its strong oxidative properties (Monks et al., 2015). While O<sub>3</sub> in the lower atmosphere is predominantly produced through photochemical reactions, stratospheric intrusions (SIs) – the process where O<sub>3</sub>-rich air masses from the stratosphere descend to the lower troposphere – can also increase surface O<sub>3</sub> concentrations in certain regions (Akritidis et al., 2018; Škerlak et al., 2019; Dreessen, 2019). The natural SI processes complicate efforts to manage and reduce anthropogenic O<sub>3</sub> pollution (Zhao et al., 2025). Therefore, understanding how SI affects surface O<sub>3</sub> is crucial for improving strategies to mitigate O<sub>3</sub> pollution.</p>
      <p id="d2e374">SI is a key component of extratropical weather processes, and detecting SI events and their influence on tropospheric chemistry has been a major scientific concern across Europe (Appenzeller and Davies, 1992; Stohl et al., 2003; Akritidis et al., 2018), North America (Hocking et al., 2007; Lin et al., 2016; Wang et al., 2020b), East Asia (Lin et al., 2021; Liu et al., 2024; Chen et al., 2024), and other extratropical regions (Zhang et al., 2024). Numerous evidence has shown that surface O<sub>3</sub> concentrations can episodically rise during the SI events (Cristofanelli et al., 2010; Langford et al., 2012; Yates et al., 2013; Lin et al., 2015; Dreessen, 2019; Ou-Yang et al., 2022; Chen et al., 2023; Chen et al., 2024). In previous studies, balloon-based ozonesondes generally served as a key tool for identifying the SI events since it provides complete O<sub>3</sub> profiles up to approximately 35 km. However, the detailed structure of stratospheric O<sub>3</sub> intrusion into the surface layer remains poorly understood due to limited ozonesonde measurements at both temporal and spatial scales (Chen et al., 2011; Zhao et al., 2021; Hong et al., 2024). Consequently, the SI contribution to surface O<sub>3</sub> has long been a topic of much debate over the past few decades (Stohl et al., 2003; Yang et al., 2022; Zheng et al., 2024). Up to now, much of the understanding of SI and its contribution to surface O<sub>3</sub> pollution comes from satellite observations (Li et al., 2015; Zhang et al., 2022; Jaeglé et al., 2017), atmospheric reanalysis (Chen et al., 2023; Knowland et al., 2017; Bartusek et al., 2023; Akritidis et al., 2018), and model simulations (Wang et al., 2020a; Zhao et al., 2021; Zhang et al., 2022; Chang et al., 2023; Hong et al., 2024; Luo et al., 2024; Zhao et al., 2024; Zhu et al., 2024; Škerlak et al., 2019). Due to a common dearth of validation against with ozonesonde measurements, large uncertainties existed in the abovementioned studies. On the other hand, there are some studies that try to quantify stratospheric influences using ground-based chemical tracers, e.g., the ratio of O<sub>3</sub> to CO (O<inline-formula><mml:math id="M34" display="inline"><mml:mrow><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula>) (Ma et al., 2014; Chen et al., 2024), cosmogenic sulfur (<sup>35</sup>S) (Lin et al., 2016, 2021), and the ratio of cosmogenic beryllium-10 to beryllium-7 (<inline-formula><mml:math id="M36" display="inline"><mml:mrow><mml:msup><mml:mi/><mml:mn mathvariant="normal">10</mml:mn></mml:msup><mml:mi mathvariant="normal">Be</mml:mi><mml:msup><mml:mo>/</mml:mo><mml:mn mathvariant="normal">7</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula>Be) (Jordan et al., 2003; Liu et al., 2024). Their results also have embedded uncertainties because little is known about the SI structure aloft from the ground-based measurements alone (Zheng et al., 2024). Opposite conclusions were even drawn from different chemical tracers. For example, a study using <sup>35</sup>S as chemical tracer (Lin et al., 2021) revealed a west-high–east-low SI contribution over China, whereas a study using O<inline-formula><mml:math id="M38" display="inline"><mml:mrow><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula> ratio as tracer (Chen et al., 2024) suggested an inverse distribution of SI contribution. The lack of consensus led to significant cognitive confusion, emphasizing the urgent need for direct ozonesonde observations to refine the fundamental understanding of stratospheric O<sub>3</sub> intrusion and its contribution to surface O<sub>3</sub> pollution.</p>
      <p id="d2e514">This study focuses on a typical SI event associated with a high-level trough observed over China during 10–13 June 2013. During this event, severe surface O<sub>3</sub> pollution successively occurred in the high-elevation Tibetan Plateau and low-altitude eastern China. To explore the potential linkage between the SI process and O<sub>3</sub> pollution, we combined multi-site consecutive ozonesondes, ground-based O<sub>3</sub> measurements, satellite O<sub>3</sub> products, and atmospheric O<sub>3</sub> reanalysis. Through detailed analysis of multi-source data in this SI event, this study aims to (1) characterize the spatial and temporal behavior of high-level trough-induced stratospheric O<sub>3</sub> intrusion, (2) quantify the SI contribution to surface O<sub>3</sub> pollution and (3) elucidate the underlying dynamical mechanisms.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Datasets</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Ozonesonde observation</title>
      <p id="d2e596">In China, ozonesondes, along with radiosondes, were routinely launched weekly in Beijing (39.80° N, 116.47° E) and Hong Kong (22.31° N, 114.17° E). During June 2013, an intensive ozonesonde launch experiment was held in Beijing and Changchun (43.90° N, 125.20° E), with consecutive launches from 10 to 13 June. The details of the intensive experiment can be found in Zhang et al. (2013). These sondes (including the routine ozonesonde in Hong Kong) were launched around 13:30 China Standard Time, providing high-resolution profiles of O<sub>3</sub> partial pressure, atmospheric pressure, temperature, and humidity from the surface up to approximately 35 km (Zhang et al., 2021; Liao et al., 2024). For this study, data from nine ozonesonde observations were analyzed to examine stratospheric O<sub>3</sub> intrusion during 10–13 June 2013, including 4 consecutive days in Beijing and Changchun, and a single launch on 13 June in Hong Kong. By comparing the sonde-based surface O<sub>3</sub> concentrations with ground-based O<sub>3</sub> measurements (Fig. 3b), we demonstrated good accuracy of these ozonesonde observations (<inline-formula><mml:math id="M52" display="inline"><mml:mrow><mml:mi>R</mml:mi><mml:mo>=</mml:mo></mml:mrow></mml:math></inline-formula> 0.981 and MAB <inline-formula><mml:math id="M53" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 3.2 ppbv).</p>
</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>Atmospheric reanalysis data</title>
      <p id="d2e661">ERA5, the fifth-generation ECMWF (European Centre for Medium-Range Weather Forecasts) global reanalysis, offers a comprehensive dataset at a spatial resolution of 0.25° <inline-formula><mml:math id="M54" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.25° and a temporal resolution of 1 h for climate and weather analysis (Hersbach et al., 2020). It integrates model data with observations using four-dimensional variational assimilation in ECMWF's Integrated Forecast System (IFS). This study utilized ERA5 data, including geopotential height, potential vorticity, and wind fields, to describe the synoptic conditions during the stratospheric intrusion event.</p>
      <p id="d2e671">EAC4 (ECMWF Atmospheric Composition Reanalysis 4) represents the fourth generation of ECMWF's atmospheric composition reanalysis, with a spatial resolution of 0.75° <inline-formula><mml:math id="M55" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.75° and a temporal resolution of 3 h (Inness et al., 2019). EAC4 assimilates data from various satellite sources, including total column O<sub>3</sub> from the Ozone Monitoring Instrument and Global Ozone Monitoring Experiment-2 on MetOp satellites, profile data from the Microwave Limb Sounder, and partial columns from Solar Backscatter Ultra-Violet and Ozone Mapping and Profiler Suite. Note that surface O<sub>3</sub> measurements and ozonesonde O<sub>3</sub> profile data in China are not assimilated into the EAC4 reanalysis. The IFS used in EAC4 incorporates an extended version of the Carbon Bond 2005 chemical mechanism, which includes 126 tropospheric reactions. The emission datasets are composed of anthropogenic emissions from the MACCity inventory (Granier et al., 2011), biogenic emissions from the MEGAN2.1 model (Guenther et al., 2006), and biomass burning emissions from the Global Fire Assimilation System (Kaiser et al., 2012). Apart from O<sub>3</sub>, the stratospheric O<sub>3</sub> tracer (O<sub>3</sub>S, O<sub>3</sub> originating from the stratosphere) is also provided in the EAC4 reanalysis. This study employed both O<sub>3</sub> and O<sub>3</sub>S to characterize the three-dimensional structure of stratospheric O<sub>3</sub> intrusion.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <label>2.3</label><title>Auxiliary data</title>
      <p id="d2e780">Additional data sources included ground-based O<sub>3</sub> measurements from the China National Air Quality Monitoring Network and the Hong Kong Environmental Protection Department, satellite cloud images from the Moderate Resolution Imaging Spectroradiometer (MODIS), satellite O<sub>3</sub> products from the Atmospheric Infrared Sounder (AIRS) (Aumann et al., 2003), and atmospheric O<sub>3</sub> reanalysis from the Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA2) (Gelaro et al., 2017). According to previous studies (Jaeglé et al., 2017; Knowland et al., 2017; Zhang et al., 2022), we used satellite O<sub>3</sub> retrieved from AIRS Level 3 product, which has a spatial resolution of 1° <inline-formula><mml:math id="M70" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 1°. In contrast, the MERRA2 reanalysis has a spatial resolution of 0.5° <inline-formula><mml:math id="M71" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.625°. Both AIRS and MERRA2 O<sub>3</sub> products served as alternative references to EAC4 O<sub>3</sub> reanalysis to provide a large-scale view of horizontal and vertical O<sub>3</sub> structures during the SI event. Hourly surface O<sub>3</sub> concentrations from 77 cities in China (including Hong Kong) were used to assess nationwide O<sub>3</sub> pollution during the stratospheric intrusion event.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Results</title>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Ozonesonde evidence of stratospheric O<sub>3</sub> intrusion</title>
      <p id="d2e905">Figure 1 illustrates the evolution of the upper-level trough event from 10 to 13 June 2013. On 10 June, the upper-level trough extended from the Mongolian Plateau towards the Tibetan Plateau. By 11 June, the trough had moved eastward and deepened into a “V-shaped” structure between 90 and 120° E, causing an extremely distorted westerly jet and strong northerlies at the western flank of the trough. On this day, the emerged 1.5 PVU potential vorticity contours at 400 hPa provide convincing evidence for a deep stratospheric intrusion. On 12 June, the “V-shaped” trough persisted at 200 hPa. By 13 June, the upper-level trough had weakened to be a shallow structure over the North China Plain (NCP). Three-dimensional dynamics associated with upper-level troughs involves stratospheric dry intrusion (SDI) and warm conveyor belt (WCB) airstreams (Browning and Roberts, 1994; Browning, 1997). The SDI originates in the lower stratosphere on the cold side of the trough (west of the trough axis) and descends behind the cold front, while the WCB originates in the warm sector of the trough (east of the trough axis), ascending rapidly to the middle and upper troposphere. During this event, these contrasting airstreams led to significantly different weather conditions at the two sides of the trough, with cloudy weather in the WCB zone (east) and clear weather in the SDI zone (west). There appeared an obvious transition from cloudy to clear weather in the eastern China with the eastward movement of upper-level trough. On 13 June, China, excluding the northeast and eastern coastal regions, experienced clear weather.</p>

      <fig id="F1" specific-use="star"><label>Figure 1</label><caption><p id="d2e910"><bold>(a)</bold> Horizontal distribution of geopotential height (shading, gpm), and wind direction of jet stream in excess of 20 m s<sup>−1</sup> (arrows) at 200 hPa, and potential vorticity of 1.5 PVU (blue contours) at 400 hPa. <bold>(b)</bold> MODIS satellite cloud images with the dashed box marking eastern China (21–41° N, 105–121° E). Red dot lines in panel <bold>(a)</bold> denote the axis of the upper-level trough at 200 hPa. Magenta circles in panels <bold>(a)</bold> and <bold>(b)</bold> mark the available ozonesondes at different sites (BJ: Beijing, CC: Changchun, and HK: Hong Kong) on different days.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/25/14865/2025/acp-25-14865-2025-f01.jpg"/>

        </fig>

      <p id="d2e945">Previous ozonesonde-based observational studies (Lemoine, 2004; Hwang et al., 2007; Chen et al., 2011; Ojha et al., 2017) revealed that a secondary O<sub>3</sub> peak in a height range between 9 and 16 km (i.e., near the tropopause) is a characteristic O<sub>3</sub>-profile structure when SI occurs and triggers tropopause folding. The continuous and multi-site ozonesondes in this study provided a unique opportunity to characterize stratospheric O<sub>3</sub> intrusion linked to an upper-level trough from an observational perspective (Fig. 2). On 10 June, before the trough arrived, Beijing was influenced by WCB airstreams, showing high relative humidity (<inline-formula><mml:math id="M82" display="inline"><mml:mo lspace="0mm">&gt;</mml:mo></mml:math></inline-formula> 60 %) in the upper troposphere. By 11 June, Beijing was near the trough axis, and the O<sub>3</sub>-rich SDI airstream began to affect the upper atmosphere, creating a secondary O<sub>3</sub> peak (<inline-formula><mml:math id="M85" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> 400 ppbv at 9.5 km height) just above the rapidly descended thermal tropopause (which dropped from 10.5 km on 10 June to 8.2 km on 11 June). Besides, the cold dry air of the SDI led to a quick drop in relative humidity from 70 % on 10 June to below 25 % on 11 June in the upper troposphere of Beijing. On 12 and 13 June, the secondary O<sub>3</sub> peaks continued to be observed over Beijing, with peak concentrations rising to 650 ppbv by 13 June, but the altitude of these peaks gradually increased up to 13.6 km by 13 June with the increase in thermal tropopause height. Unlike that in Beijing, the sonde-based O<sub>3</sub> profiles in Changchun showed secondary O<sub>3</sub> peak only in 13 June, when upper-level trough moved eastward to affect Changchun. However, sub-high O<sub>3</sub> layer (<inline-formula><mml:math id="M90" display="inline"><mml:mo lspace="0mm">&gt;</mml:mo></mml:math></inline-formula> 120 ppbv) appeared in the middle troposphere (4.2–8.1 km height, the shaded light gray in Fig. 2) in advance on 12 June, accompanied by extremely low relative humidity. This sub-high O<sub>3</sub> layer is likely the transport result of pre-intruded O<sub>3</sub> from stratosphere over Beijing or its surroundings. Similar sub-high O<sub>3</sub> layer (<inline-formula><mml:math id="M94" display="inline"><mml:mo lspace="0mm">&gt;</mml:mo></mml:math></inline-formula> 80 ppbv) also occurred in the lower troposphere (3.5–6.0 km height, the shaded light gray in Fig. 2) of Hong Kong (a subtropical city) on 13 June. These high-O<sub>3</sub> and low-humidity air masses in the troposphere reflect obvious stratospheric origin, suggesting a widespread SI influence from extratropics to subtropics during this deep trough event.</p>
</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><title>Three-dimensional structure of stratospheric O<sub>3</sub> intrusion</title>
      <p id="d2e1113">The multi-site ozonesonde observations only provide a snapshot of stratospheric O<sub>3</sub> intrusion. To further visualize the three-dimensional structure, we introduced the commonly used O<sub>3</sub> products, including AIRS satellite observation, MERRA2 and EAC4 reanalysis (Li et al., 2015; Knowland et al., 2017; Akritidis et al., 2018). These three large-scale O<sub>3</sub> products were firstly validated against our ozonesonde observations. As shown in Fig. 2, AIRS satellite observation missed the upper-level secondary O<sub>3</sub> peaks and the boundary layer O<sub>3</sub> enhancements. MERRA2 reanalysis captured the secondary O<sub>3</sub> peaks but still showed large negative biases to the observed boundary layer O<sub>3</sub> enhancements. In contrast, EAC4 reanalysis reproduced well the major features of the O<sub>3</sub> vertical distribution, including upper-level secondary O<sub>3</sub> peaks and boundary layer O<sub>3</sub> enhancements. Particularly, EAC4 exactly captured the SI-induced sub-high O<sub>3</sub> layers in the middle troposphere of Changchun (on 12 June) and the lower troposphere of Hong Kong (on 13 June). This qualitative comparison suggests that EAC4 had a powerful ability to reproduce both the SI dynamics and boundary layer photochemical processes. The scatter comparison with quantitative statistics in Fig. 3a further demonstrates that EAC4 O<sub>3</sub> reanalysis had the strongest correlation (<inline-formula><mml:math id="M109" display="inline"><mml:mrow><mml:mi>R</mml:mi><mml:mo>=</mml:mo></mml:mrow></mml:math></inline-formula> 0.947), the lowest mean absolute bias (MAB <inline-formula><mml:math id="M110" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 19.1 ppbv), the lowest root mean square error (RMSE <inline-formula><mml:math id="M111" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 36.9 ppbv), and the largest index of agreement (IOA <inline-formula><mml:math id="M112" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 0.985) with the ozonesonde observation. This sonde-based validation (Fig. 3a), along with validation against with nationwide surface O<sub>3</sub> observations (Figs. 3b and 5a), provides us enough confidence in adopting EAC4 reanalysis to explore the three-dimensional structure of trough-induced stratospheric O<sub>3</sub> intrusion.</p>

      <fig id="F2" specific-use="star"><label>Figure 2</label><caption><p id="d2e1278">O<sub>3</sub> vertical distribution over <bold>(a)</bold> Beijing, <bold>(b)</bold> Changchun, and <bold>(c)</bold> Hong Kong derived from ozonesonde and other data sources (including AIRS satellite observation, EAC4 and MERRA2 reanalysis) during 10–13 June 2013. Black and blue lines denote the sonde-based temperature and relative humidity profiles, respectively. Gray dashed lines represent the thermal tropopause height, and gray dot lines indicate the boundary layer top height. Upper-level secondary O<sub>3</sub> peaks are shaded heavy gray, and SI-induced O<sub>3</sub>-rich layer in the troposphere is shaded light gray.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/25/14865/2025/acp-25-14865-2025-f02.png"/>

        </fig>

      <p id="d2e1324">Figure 4 illustrates the EAC4-based three-dimensional structure of upper-level trough-induced stratospheric O<sub>3</sub> intrusions over China. High O<sub>3</sub> concentrations at 200 hPa aligned with the trough location, extending southwestward (10 June) and southward (11–13 June) along the trough axis, which explained the upper-level secondary O<sub>3</sub> peaks over Beijing since 11 June and over Changchun on 13 June well (Fig. 2a and b). The stratospheric intrusions developed into elongated (about 2000 km) and slender (about 200 km) streamers with elevated O<sub>3</sub> concentrations exceeding 150 ppbv (referred to as SDI-induced O<sub>3</sub>-rich belts) at 400 hPa. On the east of the SDI streamers, the WCB streamers were parallel with anomalously low O<sub>3</sub> concentrations (referred to as WCB-related O<sub>3</sub>-poor belts). On 12 June, the SDI-induced O<sub>3</sub>-rich belt stretched to northeastern China, explaining the observed sub-high O<sub>3</sub> layer in the middle troposphere of Changchun (Fig. 2b). In the lower troposphere (700 hPa), O<sub>3</sub>-rich air masses appeared over subtropical southern China on 11 June, the strongest SI day, indicating the southern edge of stratospheric O<sub>3</sub> intrusion. These lower-tropospheric O<sub>3</sub>-rich air masses persisted on subsequent days and were able to be captured exactly by Hong Kong's ozonesonde on 13 June (Fig. 2c). From 11 to 13 June, there was a significant northeastward transport and dispersion of O<sub>3</sub>-rich filament due to the strengthening southwesterly winds in the lower troposphere of eastern China. Through vertical and horizontal transport, lower-tropospheric O<sub>3</sub> concentrations increased by approximately 20 ppbv across eastern China, consistent with the 18 ppbv O<sub>3</sub> increase observed at 2–6 km height over Beijing, indicating widespread enhancement of lower-tropospheric O<sub>3</sub> background due to stratospheric O<sub>3</sub> intrusion and accumulation.</p>

      <fig id="F3" specific-use="star"><label>Figure 3</label><caption><p id="d2e1485"><bold>(a)</bold> Validation of AIRS, MERRA2, and EAC4 O<sub>3</sub> products with nine ozonesonde observations from Beijing, Changchun, and Hong Kong. <bold>(b)</bold> Validation of EAC4/sonde-based surface O<sub>3</sub> concentrations with ground-based O<sub>3</sub> observations. In panel <bold>(a)</bold>, AIRS, MERRA2, and EAC4 O<sub>3</sub> data were spatially interpolated to the location of ozonesonde stations. In panel <bold>(b)</bold>, ground-based O<sub>3</sub> observations across 466 sites in 76 cities were resampled to EAC4 grid (0.75° <inline-formula><mml:math id="M140" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 0.75°) for comparison with EAC4-based surface ozone reanalysis; ground-based O<sub>3</sub> observations at three neighboring sites (Tiantan site in Beijing, Daishan Park site in Changchun, and Sham Shui Po site in Hong Kong) were used for comparison with sonde-based surface ozone concentrations. <inline-formula><mml:math id="M142" display="inline"><mml:mi>N</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M143" display="inline"><mml:mi>R</mml:mi></mml:math></inline-formula>, MAB, RMSE, and IOA denote the number of statistic samples, correlation coefficient, mean absolute bias, root mean square error, and index of agreement, respectively.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/25/14865/2025/acp-25-14865-2025-f03.png"/>

        </fig>

      <p id="d2e1582">Compared with total O<sub>3</sub>, O<sub>3</sub>S provides a more direct view of stratospheric intrusion (Fig. 4b). The three-dimensional O<sub>3</sub>S structure depicts the upper-level trough-induced stratospheric O<sub>3</sub> intrusion as a sheet-like lowering of the O<sub>3</sub>S-rich layer along the western flank of the trough and an O<sub>3</sub>S-rich tongue extending southward and westward from the trough base. These features aligned well with the typical structure of extratropical stratospheric intrusion associated with tropopause folding (Bithell et al., 1999; Hocking et al., 2007). On 10 June, stratospheric O<sub>3</sub> intrusion directly hit the Tibetan Plateau, triggering extremely high surface O<sub>3</sub> concentrations. From 11 to 13 June, the O<sub>3</sub>S-rich tongue progressed eastward into eastern China with the trough's eastward movement. Unlike that on the Tibetan Plateau, the O<sub>3</sub>S-rich tongue in eastern China was blocked in the lower free troposphere and did not further intrude the surface layer. This result agreed well with the observed sub-high O<sub>3</sub> layer at 3.5–6.0 km height over Hong Kong (Fig. 2c), suggestive of no direct stratospheric O<sub>3</sub> intrusion to the surface in the low-elevation eastern China. Nevertheless, these O<sub>3</sub>-rich stratospheric air masses can be further transported into atmospheric boundary layer via convective mixing pathway, contributing to boundary layer O<sub>3</sub> increase. In this process, their stratospheric characteristics (high O<sub>3</sub>, low humidity) tend to be lost due to strong turbulence mixing, eventually becoming unrecognizable in atmospheric boundary layer. Interestingly, another stratospheric intrusion induced by severe tropical storm (name: “Yagi”) over the northwestern Pacific provided a parallel reference (Fig. 4b). Compared with the tropical storm-induced stratospheric O<sub>3</sub> instruction, the upper-level trough-induced intrusion descended to a relatively lower altitude, causing widespread O<sub>3</sub>S signals in the atmospheric boundary layer over eastern China. Note that apart from the trough- and storm-induced SI, a secondary SI emerged in the upwind of upper-level trough on 12 June likely driven by peripheral compensatory flows. This secondary SI led to elevated O<sub>3</sub> concentrations over the Mongolian Plateau (Fig. 4a). However, they were not further transported into eastern China.</p>

      <fig id="F4" specific-use="star"><label>Figure 4</label><caption><p id="d2e1752"><bold>(a)</bold> Spatial distribution of O<sub>3</sub> concentrations in 200, 400, 700 hPa, and surface layer. <bold>(b)</bold> Three-dimensional structure of O<sub>3</sub>S concentrations. In panel <bold>(a)</bold>, white dashed lines mark the trough axis at 200 hPa, and magenta half-circles mark the locations of ozonesondes at different sites (Beijing, Changchun and Hong Kong) on different days.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/25/14865/2025/acp-25-14865-2025-f04.png"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS3">
  <label>3.3</label><title>Stratospheric intrusion contribution to surface O<sub>3</sub> pollution</title>
      <p id="d2e1805">Figure 5a presents the spatial distribution of surface O<sub>3</sub> concentrations derived from ground-based measurements and EAC4 reanalysis during the SI event. The EAC4-based surface O<sub>3</sub> reanalysis agreed well with nationwide ground-based observations (<inline-formula><mml:math id="M167" display="inline"><mml:mrow><mml:mi>R</mml:mi><mml:mspace linebreak="nobreak" width="0.33em"/><mml:mo>=</mml:mo></mml:mrow></mml:math></inline-formula> 0.697, MAB <inline-formula><mml:math id="M168" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 12.4 ppbv, RMSE <inline-formula><mml:math id="M169" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 23.5 ppbv, and IOA <inline-formula><mml:math id="M170" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 0.961, Fig. 3b), again confirming the reliability of the EAC4 reanalysis as in the previous validation with ozonesondes. On 10 June, the Tibetan Plateau experienced high O<sub>3</sub> concentrations near or exceeding 80 ppbv, with observed O<sub>3</sub> in Lhasa reaching up to 100 ppbv at 14:00 BJT. In contrast, eastern China exhibited low O<sub>3</sub> concentrations (<inline-formula><mml:math id="M174" display="inline"><mml:mo lspace="0mm">&lt;</mml:mo></mml:math></inline-formula> 40 ppbv) due to cloudy and rainy weather on this day. From 10 to 13 June, surface O<sub>3</sub> concentrations decreased day by day on the Tibetan Plateau, while they increased from west to east in eastern China. By 13 June, eastern China suffered severe O<sub>3</sub> pollution, with observed O<sub>3</sub> concentrations exceeding 100 ppbv in most of the NCP cities. From 10 to 13 June, the continuous stratospheric dry intrusion led to a weather transition from cloudy to cloudless in eastern China (Fig. 1b), enhancing photochemical O<sub>3</sub> production due to the abundance of O<sub>3</sub> precursors over there. On the other hand, strong solar radiation in cloudless weather promoted the development of thermal convection, facilitating the mixing of pre-intruded O<sub>3</sub>-rich stratospheric air from the lower free troposphere into the surface layer. These two mechanisms combined to trigger severe O<sub>3</sub> pollution in eastern China on 13 June. The continue ozonesondes in Beijing provide convincing evidence for these two mechanisms. Returning to Fig. 2a, boundary layer O<sub>3</sub> concentrations in Beijing increased significantly from 57.8 ppbv on 10 June to 120.6 ppbv on 13 June. Considering the sharp O<sub>3</sub> gradient in the interface between the atmospheric boundary layer and the lower free troposphere, the dramatic increase in boundary layer O<sub>3</sub> can be primarily attributed to photochemical production (Liao et al., 2024). However, the concurrent rise in O<sub>3</sub> concentrations in the lower free troposphere (an 18 ppbv O<sub>3</sub> increase at 2–6 km height from 10 to 13 June) indicated that stratospheric O<sub>3</sub> intrusion contributed to elevating lower-tropospheric O<sub>3</sub> background, ultimately exacerbating boundary layer O<sub>3</sub> pollution.</p>

      <fig id="F5" specific-use="star"><label>Figure 5</label><caption><p id="d2e2033"><bold>(a)</bold> Surface spatial distribution of the total O<sub>3</sub> concentration derived from ground-based measurement (dots) and EAC4 reanalysis (shading). <bold>(b)</bold> Surface spatial distribution of O<sub>3</sub>S concentration derived from EAC4 reanalysis. <bold>(c)</bold> Spatial distribution of O<sub>3</sub>S fraction in surface O<sub>3</sub> concentration calculated from EAC4 reanalysis.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/25/14865/2025/acp-25-14865-2025-f05.png"/>

        </fig>

      <p id="d2e2087">To quantify the contribution of stratospheric intrusion to surface O<sub>3</sub> pollution, Fig. 5b illustrates the spatial distribution of EAC4-based surface O<sub>3</sub>S concentrations during the SI event, and Fig. 5c shows the contribution fraction (CF) of O<sub>3</sub>S in surface O<sub>3</sub> concentrations (CF <inline-formula><mml:math id="M198" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 100 % <inline-formula><mml:math id="M199" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> O<sub>3</sub>S/O<sub>3</sub>). The high-elevation Tibetan Plateau received a high concentration O<sub>3</sub> from stratospheric intrusion, particularly on 10 June, when the upper-level trough was oriented northeast–southwest towards the Tibetan Plateau. On this day, surface O<sub>3</sub>S concentration exceeded 30 ppbv (up to 48.5 ppbv) on the Tibetan Plateau, contributing to over 30 % of the surface O<sub>3</sub> concentration (up to 44.7 %). Subsequent days saw a gradual decrease in O<sub>3</sub>S over the Tibetan Plateau. On 12 and 13 June, significant O<sub>3</sub>S hotspots (<inline-formula><mml:math id="M207" display="inline"><mml:mo lspace="0mm">&gt;</mml:mo></mml:math></inline-formula> 20 ppbv) appeared in the Mongolian Plateau. In conjunction with the three-dimensional O<sub>3</sub>S structure (Fig. 4b), the elevated O<sub>3</sub>S concentrations in the Mongolian Plateau can be attributed to the emerged secondary SI on 12 June rather than initial trough-induced SI. It seems that the elevated O<sub>3</sub>S in the Mongolian Plateau had no influences on surface O<sub>3</sub> over eastern China considering its downwind location in the lower troposphere. Nonetheless, eastern China was affected not only by the “fresh” stratospheric air in the eastward movement O<sub>3</sub>S-rich tongue (via convective mixing), but also by the pre-intruded “aged” stratospheric air from the Tibetan Plateau (via eastward transport). Due to continuous accumulation, region-averaged O<sub>3</sub>S concentrations increased approximately 1.0 ppbv in eastern China from 10 to 13 June, whereas their fraction in surface O<sub>3</sub> decreased from 11.8 % to 8.3 % as local O<sub>3</sub> photochemical production accelerated. On 13 June, surface O<sub>3</sub>S concentrations in eastern China ranged from 3 to 15 ppbv, accounting for 2 %–10 % of surface O<sub>3</sub> concentrations. Particularly in the highly polluted NCP region, O<sub>3</sub>S contributed approximately 10 % of surface O<sub>3</sub>, reflecting a non-negligible role of stratospheric O<sub>3</sub> intrusion in exacerbating surface O<sub>3</sub> pollution.</p>

      <fig id="F6" specific-use="star"><label>Figure 6</label><caption><p id="d2e2343">Schematic illustration of upper-level trough-induced stratospheric O<sub>3</sub> intrusion influence on surface O<sub>3</sub> pollution over China.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/25/14865/2025/acp-25-14865-2025-f06.jpg"/>

        </fig>

</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <label>4</label><title>Conclusions and discussion</title>
      <p id="d2e2379">This study reveals that the upper-level trough-induced stratospheric O<sub>3</sub> intrusion over China did not occur as a local-scale vertical descent from the stratosphere to the lower troposphere just at the mid-latitude location where tropopause folding occurs; instead, it involved a long-range transport from mid-latitude tropopause folding zone (e.g., Beijing) to lower-latitude areas (e.g., Hong Kong), featuring an O<sub>3</sub>-rich “tongue” structure with upper-level secondary O<sub>3</sub> peak at the base of tongue (e.g., over Beijing) and lower-tropospheric sub-high O<sub>3</sub> layer at the tip of tongue (e.g., over Hong Kong). The O<sub>3</sub>-rich “tongue” swept through the high-elevation Tibetan Plateau when the upper-level trough extended towards this highland region at its initial stage, triggering extreme surface O<sub>3</sub> pollution. With the eastward movement of upper-level trough, the O<sub>3</sub>-rich “tongue” penetrated into the lower troposphere of low-elevation eastern China. Over there, the intruded O<sub>3</sub>-rich stratospheric air masses in the lower troposphere, including the “fresh” stratospheric air vertically transported from O<sub>3</sub>-rich “tongue” and the “aged” stratospheric air horizontally transported from the Tibetan Plateau, were then entrained into the atmospheric boundary layer via lower-tropospheric dynamic processes (e.g. convective mixing). At the same time, the strengthening lower-tropospheric southwesterly winds with the eastward movement of upper-level trough gradually participated to transport these O<sub>3</sub>-rich stratospheric air back to the mid-latitudes, ultimately exacerbating surface O<sub>3</sub> pollution in the NCP region (e.g., Beijing). While several SI events have been reported in China (Chang et al., 2023; Hong et al., 2024; Li et al., 2015; Luo et al., 2024; Wang et al., 2020a; Zhang et al., 2022; Zhao et al., 2024), this trough-induced SI episode may be the first event of its widespread impact and refined structure documented (Fig. 6).</p>
      <p id="d2e2482">The quantitative stratospheric intrusion contributions derived from the validated EAC4 reanalysis are generally consistent with previous model results in China. In the low-elevation eastern China, surface O<sub>3</sub>S concentrations were previously estimated to be in the range of 5–20 ppbv during the SI events (Wang et al., 2020a; Zhang et al., 2022; Chang et al., 2023). Our EAC4-based estimation agreed well with this range, reflecting the typical magnitude of SI contribution in the low-elevation eastern China. As for the high-elevation Tibetan Plateau, a case-based model study (Škerlak et al., 2019) revealed that stratospheric tracer concentrations at the surface reach peak values of 20 % of the imposed stratospheric value, and a month-based model study (Yin et al., 2023) suggested that 36.5 % of surface O<sub>3</sub> in the hotspot of the southern Tibetan Plateau was contributed by stratospheric O<sub>3</sub> intrusion. Our EAC4-based estimation was comparable to these fractional contributions, corroborating the potential of SI to significantly influence surface O<sub>3</sub> concentrations in this highland region. Besides, ground-based chemical tracer method had been developed to quantify the stratospheric intrusion contribution over China. While Chen et al. (2024) identified the nationwide SI-induced O<sub>3</sub> enhancement as a west-low–east-high spatial distribution pattern based on surface O<sub>3</sub> and CO observations, Lin et al. (2021) determined a west-high–east-low spatial distribution pattern of SI-induced O<sub>3</sub> contribution based on ground-based cosmogenic <sup>35</sup>S observations at the Himalayas and beyond. Our result appears to support the latter, which conforms to the common knowledge that the highland regions are more susceptible to stratospheric intrusion because of their proximity to the stratosphere (Škerlak et al., 2019; Wang et al., 2020b; Lin et al., 2021).</p>
      <p id="d2e2558">To the best of our knowledge, this study is the first to utilize continuous and multi-site ozonesondes to investigate stratospheric O<sub>3</sub> intrusion. While we acknowledge that a single case study may not be fully representative, it effectively demonstrates the value of continuous and multi-site ozonesonde measurements in enhancing our understanding of stratospheric O<sub>3</sub> intrusion phenomena. On the other hand, these continuous and multi-site ozonesondes provide a valuable and unique benchmark for examining the capacity of those commonly used O<sub>3</sub> products (including AIRS satellite observation, MERRA2 and EAC4 O<sub>3</sub> reanalysis) in characterizing stratospheric O<sub>3</sub> intrusion. Previous study indicated that MERRA2 can be used in scientific studies to identify SIs by both atmospheric dynamics and composition (Knowland et al., 2017). Here, we demonstrate that EAC4, a publicly available dataset from the European Centre for Medium-Range Weather Forecasts, performs better than MERRA2 in quantitatively characterizing stratospheric O<sub>3</sub> intrusion via comparative evaluation. Moreover, in contrast to MERRA2, EAC4 simulates full O<sub>3</sub> chemistry in the troposphere (an extended version of the Carbon Bond 2005 (CB05) chemical mechanism), allowing us to determine the influence of stratospheric O<sub>3</sub> on surface concentrations separate from photochemically produced O<sub>3</sub>. Therefore, this is a proof opening the door to detailed multiyear analyses of stratospheric O<sub>3</sub> intrusion and their quantitative contribution to surface O<sub>3</sub> over China and worldwide based on the publicly available EAC4 O<sub>3</sub> reanalysis.</p>
</sec>

      
      </body>
    <back><notes notes-type="dataavailability"><title>Data availability</title>

      <p id="d2e2676">All of the used data, excluding the ozonesonde in Beijing and Changchun, are open source. ERA5 atmospheric data are available from the Copernicus Climate Change Service (C3S) Climate Data Store accessible at <uri>https://cds.climate.copernicus.eu/</uri> (last access: 2 January 2025). EAC4 O<sub>3</sub> reanalysis data were obtained from the Copernicus Atmospheric Monitoring Service Data Store accessible at <uri>https://ads.atmosphere.copernicus.eu/</uri> (last access: 2 January 2025). The MODIS true color images are available from the NASA Earth Observations (NEO) at <uri>https://neo.gsfc.nasa.gov/</uri> (last access: 2 January 2025). The AIRS and MERRA2 O<sub>3</sub> products were obtained from Goddard Earth Sciences Data and Information Services Center accessible at <uri>https://disc.gsfc.nasa.gov/</uri> (last access: 2 January 2025). The ozonesonde data in Hong Kong were obtained from World Ozone and Ultraviolet Radiation Data Centre accessible at <uri>https://woudc.org/</uri> (last access: 2 January 2025). The ozonesonde data for Beijing and Changchun are available from the first author upon reasonable request (zhliao@ium.cn).</p>
  </notes><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d2e2716">ZL conceived the original idea, analyzed the data, and wrote the first version of the manuscript. JZ designed intensive ozonesonde experiments in Beijing and Changchun. ZM supervised the research project. All of the authors discussed the results and commented on the manuscript.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d2e2722">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="d2e2728">Publisher’s note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this paper. While Copernicus Publications makes every effort to include appropriate place names, the final responsibility lies with the authors. Also, please note that this paper has not received English language copy-editing. Views expressed in the text are those of the authors and do not necessarily reflect the views of the publisher.</p>
  </notes><ack><title>Acknowledgements</title><p id="d2e2734">We acknowledge the Copernicus Climate Change Service Climate Data Store, the Copernicus Atmospheric Monitoring Service Data Store, NASA Earth Observations, Goddard Earth Sciences Data and Information Services Center, and the World Ozone and Ultraviolet Radiation Data Centre for their data support.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d2e2739">This research has been supported by the National Natural Science Foundation of China (grant nos. 42405115, 42293321 and 42207115).</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d2e2745">This paper was edited by William Ward and reviewed by three anonymous referees.</p>
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    <!--<article-title-html>Widespread stratospheric intrusion influence on summer ozone pollution over China revealed by multi-site ozonesonde and validated EAC4 reanalysis</article-title-html>
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