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Seasonal variations in aerosol characteristics from local pollution and long-range transport at the northern tip of Taiwan

Abstract

Understanding aerosol characteristics and their influence on cloud condensation nuclei is essential for clarifying the connections between regional air pollution and global climate change. Asian continental outflows, laden with significant anthropogenic emissions, can profoundly affect local air quality. This study examines local pollution (LP) and long-range transport (LRT) events at Cape Fuguei, Taiwan’s northernmost point, during the spring and autumn seasons from 2014 to 2016. We utilized a multi-pronged approach that integrates in-situ measurements, back-trajectory analysis, and satellite observations to differentiate between LP and LRT events and assess their pollutant profiles. Our findings indicate notable distinctions: LRT events, primarily driven by northeastern winds, display higher activation ratios and lower black carbon (BC) ratios compared to LP events. Seasonal variations were pronounced, the activation ratios and geometric mean diameter show a stronger positive correlation during autumn LRT events compared to spring events, suggesting increased particle aging during transport. Wind direction played a crucial role in determining pollutant characteristics. Southwestern winds were associated with higher BC concentrations, indicative of LP sources, while northeastern winds during the autumn/winter monsoon were linked to LRT events with potentially more complex aerosol aging processes. These findings underscore the importance of considering both local and long-range sources in air quality assessments and the potential impacts of changing regional emission patterns on local air quality.

1 Introduction

Transboundary or long-range transport (LRT) of air pollution is a significant contributor to haze episodes across inland and coastal regions of Asia [1]. Typically observed from late autumn to early spring, the movement of cold high-pressure systems from Siberia, combined with northeast (NE) monsoons, facilitates the transport of polluted air masses across East Asia, affecting countries like China, Korea, Japan, and Taiwan [2,3,4,5,6,7,8]. The northern tip of Taiwan, such as Cape Fuguei, situated downstream of this continental outflow and separated by mountains, serves as a crucial point for assessing transboundary pollution during the NE monsoon season [9, 10]. These outflowing air masses often carry dust and PM2.5 (particulate matter with a diameter of 2.5 μm or smaller), which includes hygroscopic chemical compositions [11, 12]. During the NE monsoon season, air pollutants in East Asia are transmitted over long distances to Taiwan. It was found that air masses from mainland China contribute the most to PM2.5 levels in northern Taiwan, reaching up to 80% from winter to spring [13]. During the winter of 2017, it was found that the average mass fractions of SO4− and NO3− mixed within PM2.5 chemical compositions were 7 ± 13 and 11 ± 15%, respectively, while the aerosol mixing state continued to exhibit diversity even after regional pollution was transported over distances of 500 to 1000 km [14]. During the COVID-19 lockdown in China, the concentration of NO2 decreased by 24% compared to the same period in previous years, resulting in a significant reduction in PM2.5 concentrations reaching Taiwan [15, 16]. Simulation studies indicate that PM2.5 concentrations from LRT transport can peak between 45 to 100 µg m−3 during haze episodes [7, 17]. Furthermore, LRT from East Asia is frequently laden with anthropogenic sulfate and nitrate particles, particularly during the monsoon season [18]. Local pollutants may interact with these transported plumes, complicating the atmospheric mixture and contributing to secondary aerosol formation [18, 19], especially observed in northern urban areas of Taiwan [20].

Aerosol hygroscopicity plays a crucial role in influencing both regional and global climates, as it affects cloud condensation nuclei (CCN) and cloud formation processes. The hygroscopicity of aerosols depends on their chemical composition and particle size. Newly formed and aged aerosol particles can absorb organic and sulfuric vapors, enhancing their size and increasing CCN concentrations [21, 22]. Higher CCN concentrations can lead to increased cloud albedo, impacting the Earth’s radiation budget [23]. Smaller cloud droplets may inhibit low cloud formation and short-lived rainfall [24,25,26], while larger CCN can enhance precipitation in convective clouds [27]. Aerosols rich in hygroscopic materials can lower the supersaturation (SS) needed for vapor condensation, facilitating cloud droplet formation. However, measuring aerosol hygroscopicity in ambient environments remains challenging compared to laboratory settings [28]. An SS of 0.1% suggests the maximum expected influence of chemical composition, while 0.4% indicates conditions favorable for the formation of convective clouds. In contrast, an SS of 0.8% reflects a highly supersaturated environment, where nearly all aerosols are likely to activate as CCN [29]. The ambient observations made off the Californian coast have shown that in clean marine air, SS levels often surpass 1% [30]. In urban areas, aerosols with low hygroscopic materials, such as soot, can diminish overall hygroscopicity [31]. Conversely, low wind speeds (WS) can enhance moisture uptake in the presence of water-soluble inorganic ions, leading to size growth—a phenomenon known as aging [32,33,34,35]. Factors influencing aerosol hygroscopicity include chemical composition, environmental conditions, emission sources, mixing states, and aging processes. In situ measurements of aerosols'physicochemical properties are vital for understanding their hygroscopicity effects [36, 37].

The seasonal variations in aerosol characteristics and their impacts on CCN activity have been increasingly recognized as critical factors in understanding air quality and climate interactions. Research has shown substantial seasonal differences in aerosol physicochemical properties, influenced by meteorological conditions, emission patterns, and atmospheric chemistry [38]. The transition from winter to spring in East Asia is marked by frequent LRT events, while summer to autumn transitions often involve a mix of local and transported pollutants. Such seasonal shifts can lead to changes in particle size distributions, chemical composition, and hygroscopicity, ultimately affecting CCN activity and cloud formation processes [39]. Understanding these seasonal dynamics is essential for accurate climate modeling and effective air quality management.

To quantify LP and LRT pollutants, trajectory statistics and chemical transport models are commonly used. The former calculates emissions frequency based on backward trajectories, while the latter simulates emissions from specific areas. Both methods face uncertainties due to variabilities in emissions, chemical reactions, and meteorological conditions [40]. However, field measurements can provide valuable data to support these simulations. This study utilizes the spring (March to April) and autumn (October to November) seasons in a consecutive three years (2014–2016) of ground-based measurements, along with analysis of backward trajectories and aerosol optical depth (AOD) from satellite data, to characterize the CCN activation ratio (AR) and pollutant characteristics during LRT. By focusing on these transitional seasons, we aim to elucidate the complex interplay between local and long-range transported pollutants, their seasonal variations, and their impacts on CCN activity. This approach allows us to address critical gaps in our understanding of aerosol-cloud interactions in a region significantly affected by both local emissions and transboundary pollution.

2 Methods

2.1 Measurement site and instrumental set-up

Our approach to identifying and characterizing LRT and LP events combined in-situ measurements, local monitoring station data, back-trajectory analysis, and satellite observations. This multi-pronged strategy enabled a thorough assessment of air mass origins and properties at Cape Fuguei (25.30° N, 121.54° E), as shown in Fig. S1. This site is strategically positioned to monitor the influence of the Asian continental outflow on air quality [6, 41]. Taiwan's distinct seasonal meteorological patterns play a significant role; during winter and autumn, the northeastern monsoon exacerbates air pollution with increased rainfall and stronger winds. In contrast, spring and summer see a rise in LP from southern flows [14, 42, 43]. Although spring experiences orographic rain, most rainfall occurs during the plum rain season, leading to unstable weather and greater temperature fluctuations. The northeastern monsoon typically transports pollutants from Northeast Asia to Taiwan, highlighting Cape Fuguei's importance for monitoring pollution. Data collection took place in three periods: spring 2014 (Mar. 4 to Apr. 13), autumn 2015 (Oct. 26 to Nov. 12), and autumn 2016 (Oct. 17 to Nov. 30), acknowledging that emissions during these times may differ from winter patterns.

The PM2.5 mass concentration was measured using a Tapered Element Oscillating Microbalance (TEOM, Model 1405 F, Thermo Fisher Scientific) operating at a flow rate of 16.67 L min−1. A 7-wavelength Aethalometer (AE33, Magee Scientific, USA) was employed to directly estimate the black carbon (BC) mass concentration with aerodynamic diameter of 2.5 μm at measurement wavelength of 880 nm. The particle number size distribution was determined using a scanning mobility particle sizer (SMPS, Model 3936, TSI), which was equipped with an electrostatic classifier and a butanol-based condensation particle counter (Model 3010, TSI). The geometric mean diameter (GMD) and BC ratio were identified in Eqs. (1) and (2):

$$\text{GMD}\left({d}_{g}\right)=\text{exp}\frac{{\sum }_{i}(ln{d}_{pi})\times {N}_{i}}{{\sum }_{i}{N}_{i}}$$
(1)
$$\mathrm{BC}\;\mathrm{ratio}\;(\%)=\frac{BC\;mass\;concentration}{PM_{2.5}mass\;concentration}\times100$$
(2)

In addition, the CCN activity was assessed with a CCN counter (CCNc-100, DMT) at a flow rate of 0.5 L min−1. The AR, which signifies changes in aerosol hygroscopicity potentially influenced by particle size and composition, was computed using the number concentrations of condensation nuclei (\({N}_{CN}\)) and CCN (\({N}_{CCN}\) measured at the SS of 0.4%), as demonstrated in Eq. 3. We chose 0.4% SS as it represents a typical value for aerosol particles activated as CCN, allowing researchers to study the behavior of these particles under conditions similar to those found in natural clouds [38]. An increase in the AR value signals a higher likelihood of CCN formation. A more hygroscopic particle corresponds to a smaller activation energy barrier necessary for particle growth — conversely, particles with weaker hygroscopicity yield lower AR values.

$$AR=\frac{N_{CCN}}{N_{CN}}\times100\%$$
(3)

2.2 Multi-criteria approach for identifying LRT events

We employed a comprehensive, multi-criteria approach to robustly identify and distinguish between LRT and LP events. This strategy integrates several methods, including analysis of gaseous pollutant variations, back-trajectory modeling, and AOD observations, to address the complexities inherent in identifying pollution sources in a coastal environment influenced by both continental outflows and local emissions. The methodologies of back-trajectory and AOD analysis by using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model and the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) are shown in Text S1 and S2.

2.3 Observation of gaseous pollutant variation

The atmospheric lifetime of gaseous pollutants varies based on their physical and chemical properties, as well as the complex sources and reactions involved [44]. To identify potential LRT events, we examined the temporal variations of nitrogen oxides (NOx) and O3. The strong negative correlation between NOx and O3 diurnal patterns may indicate local sources affecting NOx levels, while a positive correlation during other times may suggest the influence of long-range transported O3 [45]. Events with minimal diurnal variations in these pollutants were flagged as potential LRT candidates. We defined non-LRT events as those with significant fluctuations in NOx and O3 levels, characterized by decreased NOx and increased O3 during the day due to photochemical reactions.

We also analyzed NOx/CO ratios, as lower ratios may indicate LRT events, given the differing atmospheric lifetimes of these species [45]. Carbon monoxide can persist for up to two months during LRT events due to its low reactivity [46], while NOx has a much shorter lifetime (6 to 21 h) and contributes to O3 formation through reactions with volatile organic compounds (VOCs) [47]. Ground-based trace gas concentration data were obtained from Taiwan EPA monitoring stations in Wanli (25.18° N, 121.69° E), representing LP at Cape Fuguei. Acknowledging the limitations of NOx/CO ratios, particularly in coastal settings, we applied additional criteria to refine our classification.

3 Results and discussion

3.1 LRT events during 2014–2016

Figure 1 illustrates the identification of LRT events based on O3 and NOx trends at the Wanli air quality station (20 km away from Cape Fuguei). Under normal conditions, O3 and NOx exhibit a clear diurnal anti-correlation due to photochemical reactions. O3 levels rise during the day as a result of these reactions, while at night, O3 decreases and NOx increases owing to the reaction between NO2 and O3. This diurnal pattern is typical in the absence of LRT. However, during transboundary pollution events, the diurnal variation of O3 diminishes, weakening its correlation with NOx. A significant anti-correlation thus serves as an indicator to differentiate between LRT and LP events. The relationship between the diurnal patterns of NOx and O3 has been extensively analyzed using functional data analysis to explore the dynamics of their cycles, interconnections, and varying spatio-temporal patterns [48]. Additionally, Zheng et al. employed the Weather Research and Forecasting-Community Multiscale Air Quality model and HYSPLIT model to simulate the formation, transport, and sources of ozone. Their findings indicate that ozone precursors emitted from northern China, South Korea, and Japan can be carried via the East China Sea to the southeastern coastal regions of China, resulting in significant transport-related ozone pollution [49].

Fig. 1
figure 1

Temporal variation of PM2.5, rainfall, GMD, AR, NOx, O3, CO and wind direction during (a) 2014 Spring, (b) 2015 Autumn, and (c) 2016 Autumn. The green area indicates LRT events

In Spring 2014, four LRT episodes were noted (Mar. 5–9, Mar. 13–15, Mar. 20–22, and Mar. 30–Apr. 6), as shown in Fig. 1a. These events did not consistently coincide with high pollution levels; for instance, average PM2.5 concentrations during Mar. 5–9 and Mar. 20–22 remained below 20 μg m−3, likely due to dilution from clean oceanic air or rainfall. Backward cluster analysis from Mar. 10–16 revealed significant air mass descent, transporting pollutants from the eastern China Sea to Cape Fuguei on Mar. 14–15 (see Fig. 2a and Fig. S2). AOD results, reaching 1.5–2 over the eastern China Sea, further support continuous pollutant transport to southern Taiwan (see Fig. 3). Although the trajectories during Mar. 10 and 12 did not indicate direct transport from high-emission areas, they represented LRT influenced by anthropogenic emissions. The mixing and transformation processes during transport can create distinct air masses, differing from fresh continental and clean marine air. Notably, on Mar. 16, there was a sharp increase in gaseous and particulate pollutants (see Fig. 1a). Analysis of surface and 925 hPa high fields indicated north and southwest (SW) winds (Fig. S3), suggesting a complex mixing event involving both LP and LRT from central to northern Taiwan.

Fig. 2
figure 2

HYSPLIT backward trajectory in two different years into Cape Fuguei (a) Mar. 10 to Mar. 16, 2014, and (b) Nov. 02 to Nov. 08, 2015

Fig. 3
figure 3

AOD results of MERRA-2 model during 00UTC, 06UTC, 12UTC, and 18UTC at (a) Mar. 14, (b) Mar. 15, and (c) Mar. 16, 2014

In Autumn 2015, three LRT events were observed (Oct. 25–28, Oct. 31–Nov. 3, and Nov. 9–11), with mean PM2.5 concentrations of 24, 17, and 21 μg m−3, respectively. A significant pollution episode occurred from Nov. 2–3, supported by backward trajectory analysis showing air mass movement from the eastern China Sea to the site (refer to Fig. 2b and Fig. S4). AOD ranged from 0.5 to 1 (the green area in Fig. S5) confirmed pollutant presence near China's eastern area. Additionally, Fig. S6 shows high PM2.5 accumulation in central Taiwan on Nov. 6–7, driven by a leeward eddy, contributing to pollution on Nov. 8, even during non-LRT days (see Fig. 1b). In Autumn 2016, four more LRT events were recorded (Oct. 29–Nov. 3, Nov. 8–11, Nov. 15–16, and Nov. 22–29). Except for Nov. 15–16, these periods experienced frequent rainfall, resulting in PM2.5 concentrations generally below 20 μg m−3 (Fig. 1c).

3.1.1 Categorization of LP and LRT events with NOx/CO correlations

Gaseous pollutants exhibit varying atmospheric lifetimes, which significantly affect their ambient concentrations and dispersion distances. For instance, NOx and CO have lifetimes ranging from 6 to 21 h and approximately 2 months, respectively, making them useful indicators for LP and LRT events [46, 50]. We hypothesized that the NOx/CO ratio during LP events, influenced by SW winds, would be higher than during LRT events associated with NE winds.

Our analysis revealed two distinct clusters in the data (see Fig. 4): one aligned with LP and the other indicating foreign transport. We recognize that the NOx/CO ratio is affected by ventilation conditions, particularly wind speed. Our findings indicate that higher NOx/CO ratios in LP cases often correlate with lower WS, which facilitate the accumulation of locally emitted pollutants. Indeed, the NOx/CO ratios for LP events were consistently higher than those for LRT events in both spring and autumn, supporting our hypothesis. Additionally, LP events were characterized by increased BC mass concentrations.

Fig. 4
figure 4

Correlation between CO and NOx against BC concentration for determining the LRT in (a) 2014 Spring, (b) 2015 Autumn, and (c) 2016 Autumn. SW: southwest wind, and NE: northeast wind. (RMSE: root mean square deviation)

In contrast, during LRT events with NE winds, the NOx/CO ratio remained around 25, accompanied by relatively low BC emissions. The distribution of the NOx/CO ratio in the autumns of 2015 and 2016 (marked by green dots in Fig. 4) suggests that air mass outflow during the winter/autumn monsoon effectively dilutes local emissions. These relationships between primary emitted NOx, CO, and BC further substantiate our classification of LRT events based on temporal variations in NOx and O3. However, distinguishing between LP and LRT events based on gas lifetimes carries inherent uncertainties due to factors like traffic intensity, relative humidity, temperature, solar radiation, and rainout effects. NOx concentrations suppress the surface O3 at night and in the early morning, leading to reduced O3 levels through chemical reactions. Vertical mixing affects the ratio of O3 precursors in the Planetary Boundary Layer by transporting near-surface O3-precusors emissions (NOx and VOCs) to higher levels. While NOx decreases rapidly with altitude, VOCs can persist longer, altering the VOC/NOx ratio and influencing O3 production [51, 52]. Despite these challenges, our simplified approach provides valuable insights into the seasonal patterns of air pollution at Cape Fuguei. Notably, the NOx/CO slope for LP events differed between Spring 2014 and Autumn 2015 but was closer to that of Autumn 2016, potentially reflecting changes in local emission sources and variations in traffic activity.

3.1.2 Case studies of LRT events

The NE wind was generally linked to LRT events, while the SW wind was associated with LP events. This study further examines the effects of transboundary pollution on AR, BC ratio, and GMD over a three-year period. Selected cases from Spring 2014 (Mar. 20–22, CASE I; Mar. 30–Apr. 6, CASE II) and Autumn 2016 (Nov. 22–27, CASE III) are analyzed based on O3-NOx temporal variation and NOx/CO ratios.

As shown in Fig. 5a, the AR, BC ratio, and GMD of CASE I ranged from 0.6–1.0, 2–6%, and 80–125 nm, respectively. Additionally, Fig. S7 illustrates an AOD distribution exceeding 1.5 along the southeastern coast of China and mainland Southeast Asia. The increased AR may be attributed to hygroscopic substances carried by oceanic air masses. In contrast, CASE II, depicted in Fig. 5b, exhibited greater fluctuations in AR, BC ratio, and GMD, with values ranging from 0.3–0.8, 1–30%, and 60–125 nm, respectively. High AOD values, as shown in Fig. S8, reached up to 2 during late March and early April, suggesting that transboundary air masses transported pollutants, evident in the significant peaks of BC ratio and GMD observed.

Fig. 5
figure 5

Time series of AR, BC ratio, and GMD during LRT. (a) CASE I, (b) CASE II, and (c) CASE III

For CASE III, Fig. 5c indicates a variation between AR and GMD, while the BC ratio consistently remained below 5%. Most air trajectories, illustrated in Fig. S9, originated from the Pacific Ocean, likely enhancing ambient relative humidity and increasing hygroscopic materials. Moreover, the average AOD, shown in Fig. S10, was less than 1, consistent with these observations. The average GMD decreased alongside AR values, ranging from 0.2 to 0.6, as highlighted in the yellow area of Fig. 5c. This suggests that the physical and chemical properties of aerosol particles affecting AR during LRT events are influenced by the winter/autumn monsoon. Thus, seasonal variations in the BC ratio and GMD may serve as indicators of pollution episodes in spring and autumn. Given that CASE III in 2016 was a notably clean LRT event, the following section will focus on comparing LRT events from Spring 2014 and Autumn 2015.

3.2 Analysis of pollutants'characteristics

3.2.1 BC ratio and AR

The relationship between the BC ratio, AR, and wind patterns offers vital insights into pollution events at Cape Fuguei. Figure 6 presents wind rose plots illustrating AR distribution and BC mass concentration for spring 2014 and autumn 2015.

Fig. 6
figure 6

AR and BC concentration against wind speed and direction at (a) 2014 Spring and (b) 2015 Autumn

In spring 2014 (see Fig. 6a), dominant eastern winds with high WS were observed. The maximum AR value of 0.8 occurred with WS between 6 to 8 m s−1, primarily from NE and east wind directions. Areas near Cape Fuguei, characterized by robust east and NE winds, frequently exhibited elevated AR values. This suggests that the strong easterly winds may have transported hygroscopic particles, potentially of marine origin, thereby enhancing CCN activity. In contrast, during autumn 2015 (see Fig. 6b), AR values ranged from 0.8 to 0.9 under NE WD, with WS varying from 2 to 8 m s−1. This pattern is attributed to the prevailing winter/autumn monsoon in northern Taiwan. The consistently high AR values across varying WS indicate that the NE monsoon significantly contributes to transporting particles with high CCN potential, likely due to the abundance of sea salt aerosols in marine-influenced air masses.

Notably, BC mass concentrations showed an inverse relationship with AR during both spring and autumn. This trend implies that non-hygroscopic materials like BC may reduce overall AR. The average AR of 0.5–0.8 observed at Cape Fuguei significantly exceeded the AR values of 0.24 ± 0.16, 0.4 ± 0.06, 0.43–0.74, 0.4–0.6, and 0.27–0.36 recorded at various coastal sites, including San Paulo [53], Shanghai [54], west coast of South Korea [55], California [56], and the eastern Arabian Sea near the southern tip of India [57]. This suggests a potentially higher level of CCN activity in our study area. Further analysis, depicted in Fig. S11 and Table S1, shows that BC ratios during LRT events were generally lower than those during non-LRT events. A negative correlation between BC ratio and AR was noted during both event types in spring 2014 and autumn 2015, highlighting the influence of aerosol composition on CCN activity. An exception occurred in autumn 2016, where a positive correlation between BC ratio and AR emerged, likely due to frequent rainfall that scavenged aerosol particles during the active monsoon season, altering the typical BC and CCN relationship.

3.2.2 Seasonal variations in pollutant characteristics

As shown in Table 1, the mean mass concentrations of PM2.5 and BC, PM2.5/PM10 and BC/PM2.5 ratios were consistently higher in spring 2014 compared to autumn 2015. This seasonal difference can be attributed to variations in meteorological conditions and pollution sources.

Table 1 Mean values and SD of WS, AR, PM2.5, PM2.5/PM10, BC, and BC/PM2.5 during 2014 spring, 2015 autumn, and 2016 autumn

In Spring 2014, when WS are generally lower, local pollutants may accumulate, leading to higher average PM2.5 and BC concentrations reached to 28.8 ± 16.6 μg m−3 and 1.01 ± 0.767 μg m−3. Generally, the elevated BC mass concentration observed during periods of lower WS (2–4 m s−1) likely represents LP, possibly generated by ship engine combustion or local burning near Fuji Harbor and carried by SW winds. Ship emissions are a source of various air pollutants, including SO2, NOx, and PM2.5, with particulate matter primarily found in smaller sizes under 0.4 μm [58]. This particulate matter mainly consists of elemental carbon, sulfates, and trace metals such as vanadium, nickel, iron, and calcium, and notably, ship emissions contribute to 5.9% of PM2.5 concentrations [59]. In contrast, during the autumn seasons of 2015 and 2016, the NE monsoon carried transboundary air masses that effectively diluted and dispersed local pollutants. The continental Asia outflow influenced the chemical composition of PM2.5, although the concentrations of these pollutants tended to decrease due to long-distance transport. Consequently, the average recorded concentrations were notably lower, with PM2.5 mass concentrations of 20 ± 12 μg m−3 in 2015 and 14 ± 8 μg m−3 in 2016. Meanwhile, BC mass concentrations were 0.7 ± 0.5 μg m−3 in 2015 and 0.7 ± 0.8 μg m−3 in 2016. The discrepancy between seasons further emphasizes the critical role of WS and direction in the distribution and characteristics of pollutants at our study site. The observed differences between spring and autumn LRT events may be partially attributed to seasonal variations in emissions across East Asia. Autumn, being a transitional season, may capture a mix of emission patterns characteristic of both summer and winter, potentially influencing the composition and properties of long-range transported aerosols. This seasonal variability in emissions, coupled with the changing meteorological conditions, likely contributes to the distinct characteristics of LRT events observed in spring versus autumn.

3.2.3 Effect of wind direction on pollutant characteristics

Wind direction significantly influences pollutant characteristics at Cape Fuguei. Figure 7 depicts the relationship between AR, BC ratio, and GMD during LRT events under prevailing NE winds in spring 2014 and autumn 2015.

Fig. 7
figure 7

Correlation of (a) AR with BC ratio in spring, (b) AR with GMD in spring (c) AR with BC ratio in autumn, and (d) AR with GMD in autumn for northeast wind

In spring 2014, LRT events exhibited typical AR values ranging from 0.6 to 0.8, generally surpassing those seen during non-LRT events. However, no significant correlation was found between AR and BC ratio (Fig. S12a) or AR and GMD (Fig. S12b) during LRT, indicating that hygroscopicity was not strongly influenced by particle size. Conversely, autumn 2015 revealed a different pattern: LRT events had higher AR values up to 0.8 to 0.95 compared to non-LRT episodes around 0.5 (Fig. 7c and d), and a positive correlation between AR and GMD was observed (Fig. 7d), with GMD values reaching up to 110 to 130 nm, larger than those (e.g., 90–100 nm) in spring 2014 (Fig. 7b). Notably, this season also showed a negative correlation between GMD and BC ratio (see Fig. S12). These seasonal variations suggest distinct aging processes for transported aerosols, with the stronger positive correlation in autumn indicating that larger particles acted as more effective CCN, likely due to enhanced aging and mixing during transport.

Our analysis of air mass back trajectories over three years indicated multiple transport pathways during winter and autumn, reflecting diverse pollutant sources during LRT events. As shown in Table S2, air masses from coastal China constituted 76% of trajectories in spring 2014, but decreased to 56 and 33% in autumns 2015 and 2016, respectively. This shift likely contributes to the observed differences in aerosol characteristics between spring and autumn. The broader distribution of GMD, coupled with heightened AR values in autumn 2015, indicates a nuanced and heterogeneous aging process (Fig. S13). This rise in GMD can likely be linked to the formation and aggregation of secondary inorganic and organic aerosols onto existing particles, alongside the aging of carbonaceous aerosols, which leads to an increase in particle size. Furthermore, this phenomenon suggests that pollutants from remote sources experience considerable transformations, leading to larger particles and increased CCN activity, especially during LRT events in the autumn. In summary, our findings highlight intricate interactions between local and long-range transported pollutants, demonstrating significant seasonal variations influenced by wind direction at Cape Fuguei.

4 Conclusions

Our study at Cape Fuguei, Taiwan’s northernmost point, sheds light on the intricate dynamics of local and LRT air pollution. By analyzing data across three seasons, we identified key differences between LP and LRT events, emphasizing the influence of meteorological conditions on air quality in this coastal area. LRT events, primarily driven by northeastern winds, consistently showed higher AR and lower BC ratios than LP events. This pattern suggests that long-distance air masses undergo transformations that enhance their role as CCN while diluting primary pollutants like BC. Notably, autumn LRT events exhibited a stronger correlation between AR and GMD compared to spring, indicating more significant aerosol aging influenced by winter and autumn monsoon conditions.

Our multi-criteria approach for identifying LRT events—combining gaseous pollutant mixing ratios, back-trajectory analysis, and AOD data—proved effective. We defined LRT events based on criteria such as minimal diurnal variations in NOx and O3, low NOx/CO ratios, back-trajectories from the Asian continent, and increased AOD along the trajectory. Despite our comprehensive approach, the complexities of a coastal environment—such as vertical pollutant transport, local marine sources, and air mass mixing—pose challenges in event classification.

Our findings highlight the necessity of considering large-scale atmospheric circulation patterns in assessing coastal air quality affected by continental outflows. Future research should focus on the chemical composition of aerosols during LRT events and the mechanisms behind seasonal variations. Long-term monitoring will be vital for evaluating trends in LRT's impact on local air quality amid shifting global emissions. Integrating our insights into regional air quality models could improve predictive capabilities, particularly in areas experiencing complex transport dynamics. Enhanced identification of LRT events could benefit from on-site measurements of a wider array of chemical species and vertical profile data, reducing uncertainties in understanding local and long-range pollutant interactions.

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Declaration of generative AI and AI-assisted technologies in the writing process

During the preparation of this work, the author(s) used OpenAI chatGPT in order to improve readability and language. After using this tool/service, the author(s) reviewed and edited the content as needed and take(s) full responsibility for the content of the publication.

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This work was financially supported by the Taiwan Ministry of Science and Technology (now the National Science and Technology Council) under grant No. MOST 105–2119-M-008–014, MOST 106–2111-M-008–009, MOST 107–2628-M-008 -002 -MY2, and NSTC 113–2222-E-110 -003 -MY2.

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Tse-Lun Chen: Conceptualization, Formal analysis, Data curation, Investigation, Writing—original draft. Wei-Jen Hsieh: Methodology, Investigation, Writing—original draft. Hsin-Chih Lai: Methodology, Data curation. Neng-Huei Lin: Conceptualization, Project administration, Supervision. Si-Chee Tsay: Methodology, Supervision. Charles C. K. Chou: Supervision. Ta-Chih Hsiao: Conceptualization, Writing -review & editing, Project administration, Supervision.

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Chen, TL., Hsieh, WJ., Lai, HC. et al. Seasonal variations in aerosol characteristics from local pollution and long-range transport at the northern tip of Taiwan. Sustain Environ Res 35, 12 (2025). https://doiorg.publicaciones.saludcastillayleon.es/10.1186/s42834-025-00250-4

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