LCM dependency on RH
Figure 1 illustrates air conditioning in the case of BAM and LCM under high RH. Since the PM2.5 concentration, due to ambient moisture and hygroscopicity, may be uncertain, the BAM maintains dry conditions by evaporating water with a heater at the inlet [29, 49]. PM2.5 concentration is precisely determined by beta-ray attenuation immediately after moisture has been removed from the sampled air. Conversely, the LCM detects light scattering by hygroscopic particles under high RH, which causes bias unless the LCM has undergone repeated calibration correctly.
To validate the model, LCM field testing was conducted over seven months, from March 25 to October 26, 2019, in Jeju, and over 22 months, from December 1, 2020, to September 30, 2022, in Singapore (Figure S4–S6 and Table S5). Figure 2 shows the PM2.5,concentrations by LCM, during high and low RH in the cases of Jeju and Singapore without post-processing calibration. Field measurements in Jeju comprised of 2,218 hourly observations over seven months. 15297 observations were made in Singapore over a period of 22 months. While comparing high and low RH, the slope in the high RH case was greater than that in the low RH, both in Jeju and Singapore (1.33 and 1.10, respectively, for high RH). In terms of regional differences, measurements had a negative zero drift tendency in Jeju, whereas they had little zero drift tendency in Singapore. These results indicate that the sensor located in a more humid climate tends to yield a higher mass concentration, showing a bias between the reference station and the low-cost sensor under high RH. Therefore, the two different instruments in Fig. 2 represent the characteristics of the BAM and LCM in relation to Fig. 1, implying that the LCM without the inlet heater results in an increased bias under high RH conditions.
Airport and LCM in relation to light scattering
LCMs operate based on light scattering; accordingly, airport visibility is evaluated based on a light scattering sensor and optical observations of aerosols around the airport, hourly or at more frequent intervals [40]. RH and PM2.5 concentrations were the most correlated parameters with visibility (Figure S3). The reported airport visibility and air quality data can elucidate the differences between the high and low RH cases during the LCM operation.
Figure 3 shows an illustrated flowchart of the calibration by the multivariate Tobit model of the airport weather and PM2.5 concentration data to correct the LCM measurements under high RH, where the LCM sample scatters light from the transmitter, and the detector estimates the mass concentration from changing a signal such as voltage in response to the scattered light. Because hygroscopic particles scatter more light under humid conditions, light scattering and electrical signal reductions should be calculated if the RH is adjusted between 30% and 40% (the low-RH case was set to 35% in the selected model). Multi-annual airport weather observations were used for training and estimating the effect of RH on light scattering, and the result was applied to the calibration process.
A visibility prediction model was built using weather observations and PM2.5 concentration data from Incheon and Jeju in Korea and Singapore. The details of each model are presented in Tables S2 and S3, and the subsequent results are provided in Table S4. Won et al. [50] showed that visibility prediction that considers PM2.5 concentration, meteorological parameters, and their relationships improved compared to other existing models. From the relationships between PM2.5 hygroscopicity, the visibility, and the extinction coefficient, airport observations and LCM measurements can be related to the hygroscopicity of PM2.5, which depends on RH. Reduced visibility under high RH indicates increased light scattering and absorption, which means an increased signal from aerosol particles under high RH, as illustrated in Fig. 3.
PM effect on light scattering depending on regional climate
Figure 4 shows the influence of air temperature (TMP), RH, and PM2.5 concentration on visibility in three different regions, which was determined by a multivariate Tobit model using airport and air quality data (the effects of all parameters on visibility estimated by the model are summarized in Table S4). In the Korean regions, RH has the most pronounced effect on visibility (-2.31 and − 2.26 km in Incheon and Jeju, respectively), followed by PM2.5 concentration (-1.00 and − 0.96 km in Incheon and Jeju, respectively), indicating that high RH and/or PM2.5 concentration is associated with decreased visibility, while TMP has a positive effect on visibility. Meanwhile, the influence of each parameter on visibility was smaller in Singapore (-0.13 km for RH) than in the Korean regions (Fig. 4a). The difference between Singapore and Korea stems from the different local climates situated at the equator and middle latitudes, respectively. In Incheon and Jeju, the TMP variation was 53°C (from − 16°C to 37°C) and 42°C (from − 6 to 36°C), while the RH variation was 90% (from 8 to 98%) and 88% (from 12 to 100%), respectively; while in Singapore, the TMP variation was 12°C (from 22°C to 34°C) and the RH variation was 57% (from 43 to 100%) during the studied period (see Table S1). TMP and RH variations are not pronounced in the equatorial region; hence, their influence on visibility may be relatively small.
Figure 4b shows an enlarged view of the effect of weather parameters on visibility; the effects of RH, WS, and PM2.5 on visibility are − 0.13 km, -0.06 km, and − 0.08 km in Singapore, respectively. Notably, unlike in Incheon and Jeju, the TMP effect on visibility is more pronounced in Singapore due to the local humid climate characteristics. The average RH during the study period was 81% in Singapore, and 62% and 67% in Incheon and Jeju, respectively (Table S1). At middle latitudes, RH variations were more pronounced than TMP variations. Conversely, at the equator, RH variation is quite small because the dew-point temperature is also relatively high, even when the TMP is high; thus, in Singapore, the influence of TMP on visibility is as pronounced as that of RH. The results from the model for the three regions reflect the similarities between neighboring mid-latitude regions and the climate characteristics at the equator.
Calibration result depending on regional models
LCM field testing combined with the calibration method was conducted in Jeju and Singapore (details are provided in Methods and Figure S5). Figure 5 shows the field measurement results for PM2.5, after applying the regional calibration by the model. Figure 5a presents the raw hourly PM2.5 concentration against the hourly measurements of the reference station, Yeon-dong, which is located near Jeju International Airport, and the other three panels present the calibrated PM2.5 concentration by the Jeju, Incheon, and Singapore models, respectively. Similar to the data in Fig. 2, raw LCM data exhibits mostly positive bias compared to those of the reference station since the PM2.5 concentration increases according to the 1.21 slope of linear regression. Conversely, low raw PM2.5 concentrations exhibit a negative bias compared to those of the reference station, indicating that the sensor has both zero and sensitivity drift in Jeju.
The three post-processed PM2.5 concentrations appear improved with linear regression slopes of 0.97, 0.98, and 1.11 respectively (Fig. 5b, 5c, and 5d). Root Mean Square Error (RMSE) is 4.7, 4.8, and 6.1 after applying the Jeju, Incheon, and Singapore models; while the Jeju model exhibits, lowest error (Fig. 5b). The Incheon model result (Fig. 5c) is almost the same as that of the Jeju model. The Singapore model result (Fig. 5d) also shows improved accuracy; nevertheless, it exhibits a tendency toward higher values compared with the Jeju and Incheon model results.
PM2.5 measurements using LCM in Singapore and the calibrated results from the three regional models are shown in Figure S8. Similar to Fig. 5, the plots from Jeju and Incheon are similar. The Singapore model result is different from the Jeju and Incheon model results, with a positive bias still remaining. It can be seen from the empirical relation stemming from the middle latitudes [46], the extinction coefficient at 80–90% RH and average PM2.5 concentration of 22 µg m− 3 is about 10–18 M m− 1 (see Methods, Eq. (3)), while a study on hygroscopicity and visibility reported a value of 5.7–7.0 M m− 1 in Singapore [51]. This difference may be reflected in the model, resulting in a more pronounced change after the calibration in Jeju than in Singapore.
Table 1
Mean PM2.5 concentration, coefficient of determination (R2), slope, RMSE, and normalized error between PM2.5 concentration measured by the LCM and measurements of the reference station over seven months (March to October 2019) in Jeju and four months (December 2020 to March 2021) in Singapore: each raw LCM value is compared with the respective calibrated values produced by three calibration methods developed by multivariate Tobit model using historical weather and air-quality data from Jeju, Incheon, and Singapore, respectively. Bold font indicates lowest errors.
|
|
Reference
Station
|
Raw
data
|
After calibration by each model
|
|
|
Jeju
|
Incheon
|
Singapore
|
Jeju
|
Mean (µg m− 3)
|
21.2
|
16.6
|
21.2
|
21.6
|
20.8
|
R2
|
|
0.85
|
0.88
|
0.88
|
0.86
|
Slope
|
|
1.21
|
0.97
|
0.98
|
1.11
|
RMSE (µg m− 3)
|
|
8.4
|
4.7
|
4.8
|
6.1
|
Normalized error (%)
|
|
33
|
17
|
17
|
22
|
Singapore
|
Mean (µg m− 3)
|
13.0
|
12.3
|
13.1
|
13.5
|
13.3
|
R2
|
|
0.51
|
0.51
|
0.53
|
0.50
|
Slope
|
|
0.91
|
0.53
|
0.56
|
0.84
|
RMSE (µg m− 3)
|
|
5.8
|
4.4
|
4.4
|
5.5
|
Normalized error (%)
|
|
33
|
26
|
26
|
31
|
All field measurement results over seven months in Jeju and 22 months in Singapore are summarized in Table 1. The average PM2.5 concentration over the measurement period in Singapore (13.0 µg m− 3) is considerably less than that in Jeju (21.2 µg m− 3). The mean PM2.5 concentration exhibits negative bias in Jeju and Singapore with 16.6 µg m− 3 and 12.3 µg m− 3, respectively. The R2 between the LCM and reference-station measurements is smaller in Singapore (0.51) than in Jeju (0.85), which may be due to the relatively low average concentration and relatively long distance between the reference station and the LCM in Singapore (Figure S5). Regarding the results after calibration by the Jeju and Incheon models, RMSEs are nearly similar (4.7–4.8 µg m− 3 in Jeju and 4.4 µg m− 3 in Singapore) while the normalized error is smaller in Jeju (17%) than in Singapore (26%). Both field experiments in Jeju and Singapore show that the mean PM2.5 concentration after calibration by the model of the same region (21.2 µg m− 3 and 13.1 µg m− 3, respectively) is closest to that of the reference station (21.2 µg m− 3 and 13.0 µg m− 3 respectively). The error of Jeju model is the lowest for field testing of Jeju and Singapore (4.7 µg m− 3 and 17%; 4.4 µg m− 3 and 26% respectively). Plots of the calibrated PM2.5 mass concentrations for different RH levels, are shown in Fig. 6. The RH and TMP-adjusted results for high RH exhibit a reduced sensor bias compared to the raw data shown in Fig. 2; the linear regression slopes of 0.91–1.02 in Jeju show that the calibration method can efficiently correct the bias of the sensor, regardless of the RH levels.
Implications of modeling for regional calibration
The present study proposes a regional LCM calibration method that estimates PM2.5, which is typically sensitive to weather, using a multivariate Tobit model with airport weather and air quality data. Instead of air conditioning to 20–23°C TMP and 30–40% RH, this method predicts PM2.5 concentration assuming that the LCM regulates TMP and RH at 21.5 ℃ and 35%, respectively. The validity of this airport weather-based calibration method was verified by constructing models for three regions, namely Incheon and Jeju in Korea at middle latitudes and Singapore at the equator, and complementary field measurements were conducted for several months in Jeju and Singapore.
The main argument against LCMs is that their accuracy is still not sufficiently high and is sensitive to the background concentration and regional environment, as also reported in the present study [16, 26, 32, 34, 35]. Although several studies have elaborated on the PM2.5 hygroscopic properties and their influence on LCM performance [26, 32, 33], other studies have reported reduced TMP and RH effects on LCM performance during field calibration [30, 52], which may be due to relatively short measurement periods, low average concentrations, and less pronounced TMP and RH variations in these regions. This study presents a novel approach for understanding regional differences by performing regional calibration using visibility-prediction models and LCM field testing in two different regions.
Considering that visibility is a simple indicator of air quality, Molnár et al. [39] showed that visibility-based PM hygroscopic growth is in good agreement with filter-based mass growth rate and can be applied to low-cost PM monitoring. Datta et al. [19] showed that a calibration equation can be applied to another LCM in the network of the region because TMP, RH, and PM2.5 concentration trends in the region are similar, which is in line with the findings of this study, which showed that the Jeju and Singapore models are most effective in field testing in Jeju and Singapore, respectively. Zusman et al. [36] showed that regional calibration may increase LCM reliability because meteorological conditions and PM sources may differ from one region to another. Onal et al. [3] showed that the IoT Big Data framework and machine learning can identify regional climate differences from complex datasets. The regional calibration method using the Tobit model with multi-annual visibility, meteorological factors, and air quality data in this study can be supported by these studies because it reflects various local factors affecting LCM performance.
Routinely correcting the bias of LCMs using filter-based mass concentrations as a reference is an easy way to increase accuracy, but this is not always applicable, as in the case of variable PM concentrations/compositions and meteorological conditions. Such a correction is also not practically feasible because of the difficult acquisition of long-term observations in all regions.
As an attempt to focus on LCM air conditioning, similar to reference instruments, and regional calibration using a multivariate Tobit model, the significance of this study is as follows. First, we showed that there is abundant data for post-processing and generating a calibration model. The multivariate model generally requires as much data as possible; and many airports and air quality authorities possess decades of weather and PM2.5 concentration data. We developed a regional calibration formula by comparing several years of airport visibility reported every hour with PM sensor measurements, showing how post-processing techniques can be applied to airport meteorological data and air quality measurements around the world. Second, we demonstrated that the calibration method can reflect local characteristics without requiring long-term field testing. The proposed method can reproduce an effect similar to that of creating empirical relations through long-term field experiments by building a visibility-prediction model using accumulated historical data. Third, the accuracy of PM monitoring, which is region-dependent, was quantified using a specific type of LCM instrument. By comparing two regions with different climate characteristics, located in the middle latitudes and equator respectively, we revealed the LCM requirements for calibration according to the local climate parameters for more reliable ambient air monitoring. LCMs still have limitations in terms of accuracy and reliability, but their potential is invaluable, when combined with advances in postprocessing methodologies [7, 8, 20].
East Asia has been experiencing increased PM2.5 concentrations due to climate change and related stagnant atmospheric conditions [53]. Southeast Asia, in particular, currently experiences severe haze every few years and faces the major challenge of mitigating any damage from such climate crises [54, 55]. Future investigations should focus on these high-impact pollution events, and the use of LCMs for this purpose should allow more communities to have easy access to air quality information. The proposed regional calibration of the postprocessing method can enhance the applicability of outdoor air quality monitoring using LCMs.