IEEE GEOSCIENCE AND REMOTE SENSING LETTERS, VOL.
19, 2022
Satellite Remote Sensing of Daily Surface Ozone
in a Mountainous Area
Songyan Zhu , Hao Zhu, Jian Xu , Member, IEEE, Qiaolin Zeng , Dejun Zhang, and Xiaoran Liu
Abstract— High levels of surface ozone (O3 ) pollution threaten
human and environmental health. Chongqing, a mountainous
municipality located in southwest China, is exposed to serious
O3 pollution and requires more studies. Due to its complex
terrain and always foggy weather, it is difficult to maintain
many in situ sites in Chongqing, and chemical transportation
model (CTM) simulations are also challenged. The recently
launched (in 2017) Sentinel-5p satellite provides O3 columns with
advanced spatiotemporal resolution. Without the dependence
on CTMs, we linked O3 columns and surface monitoring data
from 2019 to 2021 in virtue of a deep forest machine learning
model. Compared with another widely used machine learning
model and previous studies, our results showed great advantages
in estimating surface O3 on a daily scale. Validated against
in situ sites in Chongqing, averaged R 2 of cross validations
reached 0.9, while the root-mean-squared error (RMSE) and
mean bias error (MBE) were 13.57 and 0.37 µg/m3 , respectively.
We found out that the model performance is associated with
the relative height difference between training sites and the test
site. The model performed stably when the height difference was
lower than 200 m, but obvious performance degradation was seen
when the height difference is exceeding 400 m.
Index Terms— Deep forest, machine learning, mountainous
areas, O3 pollution, Sentinel-5p, TROPOspheric Monitoring
Instrument (TROPOMI).
I. I NTRODUCTION
S URFACE ozone (O3 ), one predominant air pollu-
tant in China [1], is formed through photochemical
reactions between anthropogenic/biogenic volatile organic
compounds (VOCs) and human-release nitrogen oxides
(NOx = NO + NO2). The formation pathways of O3 depend
on the ratio of the two precursors (VOCs/NOx) [2]. The O3
Manuscript received July 10, 2021; revised September 6, 2021; accepted
September 27, 2021. Date of publication October 13, 2021; date of current
version January 6, 2022. This work was supported in part by the Chongqing
Meteorological Department Business Technology Research Project under
Grant YWJSGG-202105. (Corresponding author: Hao Zhu.)
Songyan Zhu is with the Department of Geography, University of Exeter,
Exeter EX4 4RJ, U.K. (e-mail: sz394@exeter.ac.uk).
Hao Zhu, Dejun Zhang, and Xiaoran Liu are with the Chongqing Institute
of Meteorological Sciences, Chongqing 401147, China, and also with the
Chongqing Engineering Research Center of Agrometeorology and Satellite
Remote Sensing, Chongqing 401157, China (e-mail: zhuh1993@yeah.net).
Jian Xu is with the National Space Science Center, Chinese Academy of
Sciences, Beijing 100190, China (e-mail: xujian@nssc.ac.cn).
Qiaolin Zeng is with the College of Computer Science and Technology,
Chongqing University of Posts and Telecommunications, Chongqing 400065,
China, and also with the Chongqing Institute of Meteorological Sciences,
Chongqing 401147, China (e-mail: zengql@cqupt.edu.cn).
This article has supplementary material provided by the
authors and color versions of one or more figures available at
https://doi.org/10.1109/LGRS.2021.3119699.
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1004005
concentration varies by region due to many factors (e.g., mete-
orology and industrial structures). Previous studies mainly
focused on flat eastern China (e.g., North China Plain and
Yangtze River Delta) [3], [4], but the impact of terrain could
not be neglected in mountainous topography.
Mountainous southwest China has been experiencing
high levels of O3 pollution [3]. In situ monitoring [5],
satellite remote sensing [6], and chemical transportation mod-
els (CTMs) [7] are the main approaches for O3 monitor-
ing/estimation. The complex terrain causes extra challenges
in maintaining in situ sites (i.e., huge financial and labor
cost) and in modeling pollutants concentration/dispersion (e.g.,
difficulties in height layers parameterization) [8]. In addition,
studies only rely on in situ monitoring might face under-
sampling issues in capturing regional O3 variations, and the
comprehensive use of in situ and grided data could be the
solution [9], [10].
Estimating surface O3 directly from satellite column
products is an alternative solution apart from improving
CTM simulations because the latter approach requires more
advanced hardware (e.g., computer clusters), which might not
be available for all researchers across the globe [11]. Deep
learning has demonstrated the robustness in estimating air
pollution due to its complex architecture [12]. In the litera-
ture, mountainous areas were less focused on than hot-spot
areas (e.g., North China Plain) [1], [3]. For the first time,
we used a deep forest (DF21) [13] to estimate surface O3
from the TROPOspheric Monitoring Instrument (TROPOMI)
level-3 O3 columns [14] in Chongqing from 2019 to early
2021. The estimated O3 was validated against with both the
China National Environmental Monitoring Centre (CNEMC,
http://www.cnemc.cn/en/) in situ network [9] and the widely
used CTM community multiscale air quality (CMAQ) [15].
Our aim is to provide a low cost (i.e., used data and methods
are freely accessible, and the computation does not require
advanced hardware) but high-accuracy approach to monitor
regional surface O3 from space.
II. M ETHODOLOGY
A. Study Area and Data
Chongqing is a large and mountainous municipality
(82 300 km2 ) located in southwest China because about
1/3 days per year are foggy [16], which makes it more
challenging for estimating surface O3 from space. There are
17 CNEMC sites that provide hourly measured O3 mass den-
sity in µg/m3 between 2019 and 2021 (Fig. 1). The difference
1004005
Fig. 1. Distribution of CNEMC sites and mean O3 (2019–2021) columns in
Chongqing. The base map shows the terrain of Chongqing.
TABLE I
L ATITUDE /L ONGITUDE (◦ ), H EIGHT (m), AND S ITE -L EVEL O 3
M EASUREMENT OF 17 U SED CNEMC S ITES IN C HONGQING .
M EAN O 3 (O3(MN) , µ G/M3 ) I S S ITE -M EASURED M ASS D ENSITY
OF 2019–2021 AND M EAN S UMMER O 3 (O3(MNS ) , µ G/ M 3 )
I S S ITE -M EASURED M ASS D ENSITY
IN S UMMER OF 2019–2021
in height of sites could be greater than 600 m, and all sites
showed high levels of O3 pollution (Table I). For the spatial
distribution, O3 concentration in the northwest area was higher
than in the southeast part (Fig. 1). In opposite, the majority of
sites are located in the southeast area and only two sites are
in the northwest part (1414A and 1416A) (Fig. 1).
All datasets were from January 1, 2019 to January 31,
2021 because the TROPOMI Level-3 O3 product was avail-
able since late 2018. The TROPOMI Level-3 O3 product
provides global gridded (0.01◦ × 0.01◦ ) O3 columns on
a daily scale [14]. The hourly reanalyzed meteorology data
were derived from the fifth-generation atmospheric reanalyses
(ERA5) from the European Centre for Medium-Range Weather
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IEEE GEOSCIENCE AND REMOTE SENSING LETTERS, VOL. 19, 2022
Forecasts (ECMWF) [17]. ERA5 provides a large amount
of reanalyzed meteorological parameters, along with solar
radiation, fraction of cloud cover, ozone mass mixing ratio,
relative humidity, rainwater content, temperature, and U-/V-
component of wind that were used at five pressure levels
(200, 500, 700, 900, and 1000 hPa) to implicitly represent
(by nonlinear fitting) the impacts of meteorology on O3 in the
deep forest model.
B. Surface O3 Estimation Methods
1) Deep Forest: The deep forest (DF21) is an ensemble
of ensembles of decision trees [13], a cascade of tree-based
models (e.g., Xgboost [18]). Instead of using deep neural
networks (DNNs) [7], the DF21 was adopted here because
the following conditions hold [13].
1) Training DNNs requires a huge amount of data, but
DF21 exhibits great performance on small scale of
training data.
2) The architecture of DNNs could be too complicated
for many cases, but the complexity of DF21 is data-
dependent, i.e., the model complexity is automati-
cally determined by terminating training via predefined
thresholds [13].
3) The element of DF21, i.e., tree-based models, has
superior performance to DNNs on many tasks. The
features of DF21 are favorable, because for the model
of estimating surface O3 , it should be light (without
many hyperparameters and heavy dependence on CTMs)
and be off-shelf for other researchers who might be
interested in other scales/regions with limited training
data.
2) Model Implementation: The O3 columns are the integral
of O3 density along layers of height, and the ratio of surface O3
to O3 columns depends on meteorological profiles that affect
the dispersion, depletion, and transformation of O3 . The series
of O3 physical and chemical processes could be considered as
stacked nonlinear functions
   
O3(col.) = f n f n−1 · · · f 2 f 1 O3(surf.) , O3(prof.)

S R, T, R H, W(U,V ) ,Vap,cloud
where O3(col.) is the TROPOMI O3 columns, O3(surf.) is the
CNEMC surface O3 mass density, O3(prof.) is the ERA5 O3
mixing ratio profiles, SR is the solar radiation, T is the
temperature profile, RH is the relative humidity profile, W(U,V )
is the U-/V-wind component profile, Vap is the rainwater
content profile, and cloud is the cloud cover profile.
TROPOMI O3 columns and ERA5 meteorology are inputs
(i.e., explanatory variables) for model training, and the
CNEMC O3 mass density (i.e., dependent variable) is
for model validation. We adopted the leave-one-out cross-
validation (LOOCV) strategy, and therefore, we trained and
validated DF21 17 times. For each time, all data men-
tioned of 16 sites were to train the model. O3 columns and
ERA5 meteorology of the other one site were then inputted
to the trained model to get predictions. The model skill was
assessed by comparing the predictions with the CNEMC O3
mass density of the other one site. Four statistical measures
ZHU et al.: SATELLITE REMOTE SENSING OF DAILY SURFACE OZONE IN MOUNTAINOUS AREA
Fig. 2. Site-averaged DF21 estimated surface O3 (blue line) and CNEMC
measurements (orange line). The temporal resolution is three days for better
visual demonstration. Both blue and orange shadow areas represent the
intersite standard deviation.
Fig. 3. Daily site-averaged DF21 estimated, CNEMC, and CMAQ surface
O3 grouped by months.
were used for assessing the model skill: determination coef-
ficient (R 2 ), linear regression slope, root-mean-squared error
(RMSE), and mean bias error (MBE).
III. R ESULTS
Over Chongqing, DF21 reproduced the surface O3 time
series in excellent agreement with the CNEMC measurements
(Fig. 2). Seasonal patterns (e.g., summertime peaks and win-
tertime troughs) found in the CNEMC measurements were
captured by DF21 as well. The surface O3 in summer reached
around 100 µg/m3 and was around 20 µg/m3 in winter. The
O3 concentrations (i.e., mass density) in 2019 seemed higher
than those in 2020, but no obvious interannual difference
can be found from the figure. According to the narrower
shadows for the DF21 O3 time series, the intersite variations
of the DF21 results were smaller than those of the CNEMC
measurements.
The daily DF21 O3 time series agreed well with the
CNEMC measurements in all 12 months (Fig. 3). Daily scale
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TABLE II
S TATISTICAL M EASURES B ETWEEN DF21 E STIMATED S URFACE O 3 AND
CNEMC M EASUREMENTS , R 2 B ETWEEN CNEMC M EASUREMENTS
2
AND TROPMI C OLUMNS ( RC_T ), AND R 2 B ETWEEN CNEMC
M EASUREMENTS AND CMAQ E STIMATION ( RC_C 2 ). T HE U NIT
OF RMSE AND MBE I S µ G/ M 3
time series grouped by months at different years showed a
large difference, but no overall interannual pattern was seen.
It can be seen from the figure that in Chongqing, the summer
O3 was higher than that in spring and further higher than that
in autumn. In winter, when the lowest O3 was seen throughout
the whole year, the mean O3 concentration was approximately
one-third of that in summer.
Table II gives the statistical measures of DF21 validation,
R 2 between the CNEMC measured surface O3 and TROPOMI
2
columns (RC_T ), and R 2 between the CNEMC measured
2
surface O3 and CMAQ estimation (RC_C ). The first quartile
(Q1), median, and third quartile (Q3) of R 2 between CNEMC
measured and DF21 estimated surface O3 were 0.89, 0.92, and
0.94, respectively. The median of slope (of linear regression),
RMSE, and MBE were 0.97, 10.84 µg/m3 , and 4.55 µg/m3 ,
2 2
respectively. In contrast, RC_T and RC_C were low with
the median of 0.18 and 0.40, respectively. In terms of R 2 ,
the median of DF21 was 4.1 times higher than RC_T 2
and
2
1.30 times higher than RC_C . Large spatial differences in the
statistical measures were seen, especially for RMSE and MBE.
Fig. 4 shows the spatial distribution of R 2 [Fig. 4(a)] and
RMSE [Fig. 4(b)], as the slope positively correlated with
R 2 with the Pearson correlation coefficient (PCC) of 0.48
( p-value = 0.05) and the absolute MBE significantly corre-
lated with RMSE (PCC = 0.98 and p-value = 0.00). Both
panels show that the performance of DF21 was better in the
southeast Chongqing than that in the northeast Chongqing.
Site 1414A, where the elevation is about twice of other sites
on average, had the worst performance. At this site, the O3
concentration was the highest compared to other sites, and
the elevation was also the highest (600 m higher than the
nearest site 1416A and 344 m higher than the second highest
site 3015A) (Fig. 1 and Table I). Site 3015A was also seen
with large RMSE (Fig. 4(b) and Table II). On the contrary,
DF21 performed better in the southeast area, where the spatial
1004005
Fig. 4. Spatial distribution of (a) R 2 and (b) RMSE for DF21 in estimating
surface O3 . The base map shows the terrain of Chongqing.
distribution of the sites was denser, the difference in the site
height was smaller, and the overall O3 concentration was
lower.
IV. D ISCUSSION
DF21 was validated to estimate daily surface O3 with-
out dependence on CTMs. The good performance (mean
R 2 > 0.9) can be attributed to the complexity of DF21 archi-
tecture [13] and the use of hourly CNEMC O3 and meteorol-
ogy. Indicated by the importance of explanatory variables [19],
relative humidity, temperature, and cloud cover were the
most important features by separately contributing 25%, 15%,
and 10% of the importance (Table S1). This suggested that
in Chongqing, the foggy weather and clouds could heavily
affect both O3 photochemical process and model accuracy.
The performance of Xgboost validated in the same scenario
(mean R 2 = 0.8) was worse than DF21 (Table S2). In addition,
the use of DF21 is further suggested by the poor performance
(R 2 < 0.6) of 2-/8-/100-layer multilayer perceptron (MLP)
neural networks (Tables S3–S5) and the balance between
accuracy and minimum requirements of run time/hardware
(Table S6). The use of hourly data increased the size of
data by 24 times, and both DF21 and Xgboost showed better
performance than trained with daily data (Tables S7 and S8).
The use of hourly data also suggests that the DF21 can
theoretically estimate hourly surface O3 , but it can be expected
that the performance would heavily rely on the meteorology
data.
On an hourly scale, R 2 between CMAQ modeled O3 and
CNEMC measurements was lower than 0.10 at all sites.
On the contrary, the mean R 2 at daily scale increased to 0.44
(Table II), and this infers the difficulties to estimate the surface
O3 in Chongqing, especially on an hourly scale. The perfor-
mance of DF21 and Xgboost for estimating hourly surface O3
separately dropped by 8% (Table S9) and 20% (Table S10).
Therefore, we would not recommend estimating hourly surface
O3 from satellite columns, compared to previous work aiming
at improving the performance of CTM(s) [11]. In a word, for
researchers without easy in-time access to CTMs, estimating
surface O3 from satellite columns via DF21 can be a good
alternative to track O3 pollution on a daily scale.
The location of ground sites can have a significant impact
on the DF21 model performance (Fig. 4), and the high altitude
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IEEE GEOSCIENCE AND REMOTE SENSING LETTERS, VOL. 19, 2022
and/or highly polluted areas require dense distribution of
ground sites to achieve reliable performance. However, most
sites in Chongqing were operated in areas with relatively
low heights and O3 concentrations. The application here is
also beneficial to select suitable locations for future ground
sites. For instance, in Chongqing, more studies are needed to
determine the exact location and minimum number of ground
sites to guarantee the model performance.
According to the China Traffic Management Bureau
(https://122.gov.cn/), the number of vehicles in Chongqing
reached five million in April 2021, top three of all Chinese
cities. Vehicle combustion is a major source of NOx (a pre-
cursor of O3 ) [20], but measured O3 in the first four months
of 2020 was 0.5 µg/m3 per day higher than the same time
in 2019, considering the lockdown during the COrona VIrus
Disease 2019 (COVID-19) pandemic. This is different from
the situation in other areas where significant variations were
observed [21] and implies that O3 pathway in Chongqing
might be more correlated with VOCs as suggested in [22].
Future work is required to address this issue that is beyond
the scope of the current work. DF21 in estimating surface O3
in Chongqing achieves a similar performance to previous work
in other regions [21]. Considering the promising performance
despite difficulties in estimating surface O3 in Chongqing,
DF21 could potentially make a valuable contribution to the
surface O3 research in many other areas.
V. C ONCLUSION
In this study, we trained a deep forest (DF21)-based model
to estimate surface O3 concentration in a mountainous area
(Chongqing, China) from satellite observations on a daily
scale. This task is challenging considering the complex terrain
and clouds coverage in Chongqing, but the performance of
DF21 was good (R 2 = 0.9) compared to previous studies,
and the stacked “forests” outperformed single “forest” (i.e.,
Xgboost). Despite the fact that DF21 can theoretically estimate
surface O3 on an hourly scale, the results were not convincing.
The DF21 model successfully reproduced surface O3 time
series at test sites, but the performance varied spatially. The
distribution density of ground validation site network had an
important impact on the performance of DF21. Due to an
insufficient number of in situ sites in the current training,
the model performance still requires an improvement in the
regions where it has high altitude and high O3 pollution. In the
future, we will investigate the exact number and locations
of ground sites to ensure good DF21 performance, and the
application of DF21 will be extended to other areas.
R EFERENCES
[1] H. Liu et al., “Ground-level ozone pollution and its health impacts in
China,” Atmos. Environ., vol. 173, pp. 223–230, Jan. 2018.
[2] X. Jin and T. Holloway, “Spatial and temporal variability of ozone
sensitivity over hina observed from the ozone monitoring instrument,”
J. Geophys. Res., Atmos., vol. 120, no. 14, pp. 7229–7246, Jul. 2015.
[3] T. Wang, L. Xue, P. Brimblecombe, Y. F. Lam, L. Li, and L. Zhang,
“Ozone pollution in China: A review of concentrations, meteorologi-
cal influences, chemical precursors, and effects,” Sci. Total Environ.,
vol. 575, pp. 1582–1596, Jan. 2017.
ZHU et al.: SATELLITE REMOTE SENSING OF DAILY SURFACE OZONE IN MOUNTAINOUS AREA
[4] X. Lu et al., “Severe surface ozone pollution in China: A global
perspective,” Environ. Sci. Technol. Lett., vol. 5, no. 8, pp. 487–494,
2018.
[5] L. Kong, X. Tang, J. Zhu, Z. Wang, H. Wu, and J. Li, “Developing
high-resolution air quality reanalysis dataset over China for years
2013–2018 based on ensemble Kalman filter and surface observations
from CNEMC,” in Proc. EGU Gen. Assem. Conf. Abstr., 2020, p. 6848.
[6] A. H. Souri et al., “Revisiting the effectiveness of HCHO/NO2 ratios for
inferring ozone sensitivity to its precursors using high resolution airborne
remote sensing observations in a high ozone episode during the KORUS-
AQ campaign,” Atmos. Environ., vol. 224, Mar. 2020, Art. no. 117341.
[7] H. Lu et al., “Adjusting prediction of ozone concentration based on
CMAQ model and machine learning methods in Sichuan-Chongqing
region, China,” Atmos. Pollut. Res., vol. 12, no. 6, Jun. 2021,
Art. no. 101066.
[8] U. Radok, “Air pollution in the mountains,” Mountain Res. Develop.,
vol. 2, no. 4, pp. 385–389, 1982.
[9] G. Yang, Y. Liu, and X. Li, “Spatiotemporal distribution of ground-
level ozone in China at a city level,” Sci. Rep., vol. 10, no. 1, pp. 1–12,
Dec. 2020.
[10] L. Gao et al., “Comparison of ozone and PM2.5 concentrations over
urban, suburban, and background sites in China,” Adv. Atmos. Sci.,
vol. 37, no. 12, pp. 1297–1309, Dec. 2020.
[11] S. Zhu et al., “An optimization approach for hourly ozone simulation:
A case study in Chongqing, China,” IEEE Geosci. Remote Sens. Lett.,
early access, Jul. 31, 2020, doi: 10.1109/LGRS.2020.3010416.
[12] T. Li, H. Shen, Q. Yuan, X. Zhang, and L. Zhang, “Estimating
ground-level PM2.5 by fusing satellite and station observations: A geo-
intelligent deep learning approach,” Geophys. Res. Lett., vol. 44, no. 23,
pp. 11,985–11,993, 2017.
Authorized licensed use limited to: Tsinghua University. Downloaded on May 22,2023 at 02:10:51 UTC from IEEE Xplore. Restrictions apply.
1004005
[13] Z.-H. Zhou and J. Feng, “Deep forest,” 2017, arXiv:1702.08835.
[Online]. Available: http://arxiv.org/abs/1702.08835
[14] K.-P. Heue, K. U. Eichmann, and P. Valks, “TROPOMI/S5P ATBD of
tropospheric ozone data products,” Deutsches Zentrum für Luft- und
Raumfahrt (DLR), Helmholtz-Gemeinschaft, Tech Rep. S5P-L2-IUP-
ATBD-400C, 2018.
[15] M. Astitha, H. Luo, S. T. Rao, C. Hogrefe, R. Mathur, and N. Kumar,
“Dynamic evaluation of two decades of WRF-CMAQ ozone simula-
tions over the contiguous United States,” Atmos. Environ., vol. 164,
pp. 102–116, Sep. 2017.
[16] D. Liu, Z. Li, W. Yan, and Y. Li, “Advances in fog microphysics research
in China,” Asia–Pacific J. Atmos. Sci., vol. 53, no. 1, pp. 131–148,
Feb. 2017.
[17] H. Hersbach et al., “The ERA5 global reanalysis,” Quart. J. Roy.
Meteorol. Soc., vol. 146, no. 730, pp. 1999–2049, 2020.
[18] T. Chen and C. Guestrin, “XGBoost: A scalable tree boosting system,”
in Proc. 22nd ACM SIGKDD Int. Conf. Knowl. Discovery Data Mining,
Aug. 2016, pp. 785–794.
[19] L. Breiman, “Random forests,” Mach. Learn., vol. 45, no. 1, pp. 5–32,
2001.
[20] Rethinking the Ozone Problem in Urban and Regional Air Pollution,
Nat. Academies Press, Washington, DC, USA, 1992.
[21] Y. Wang, Q. Yuan, T. Li, L. Zhu, and L. Zhang, “Estimating daily full-
coverage near surface O3 , CO, and NO2 concentrations at a high spatial
resolution over China based on S5P-TROPOMI and GEOS-FP,” ISPRS
J. Photogramm. Remote Sens., vol. 175, pp. 311–325, May 2021.
[22] B. Liang, X. Yu, H. Mi, D. Liu, Q. Huang, and M. Tian, “Health
risk assessment and source apportionment of VOCs inside new vehicle
cabins: A case study from Chongqing, China,” Atmos. Pollut. Res.,
vol. 10, no. 5, pp. 1677–1684, Sep. 2019.