remote sensing

Article
Ground-Based MAX-DOAS Measurements of Tropospheric
Aerosols, NO2, and HCHO Distributions in the Urban
Environment of Shanghai, China
Haoyue Wang 1 , Wanlin Wei 1 , Huizheng Che 2,3 , Xiao Tang 4 , Jianchun Bian 5 , Ke Yu 6, * and Weiguo Wang 1

1 Department of Atmospheric Sciences, Yunnan University, Kunming 650500, China;

[email protected] (H.W.); [email protected] (W.W.); [email protected] (W.W.)
2 State Key Laboratory of Severe Weather (LASW), Chinese Academy of Meteorological Sciences (CAMS),
Beijing 100081, China; [email protected]
3 Key Laboratory of Atmospheric Chemistry (LAC), Chinese Academy of Meteorological Sciences (CAMS),
Beijing 100081, China
4 State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC),
Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China;
[email protected]
5 Key Laboratory of Middle Atmosphere and Global Environment Observation, Institute of Atmospheric
Physics, Chinese Academy of Sciences, Beijing 100029, China; [email protected]
6 Yunnan Meteorological Information Center, Kunming 650032, China
* Correspondence: [email protected]; Tel.: +86-871-6418-95-20

Abstract: Aerosol extinction profiles at 550 nm were retrieved by applying multi-axis differential
optical absorption spectroscopy (MAX-DOAS) and lookup table. Then the tropospheric NO2 and



HCHO vertical column densities were retrieved using a two-step method from 28 July to 5 August


of 2015 in Shanghai. The retrieved results were compared with the satellite products, and then
Citation: Wang, H.; Wei, W.; Che, H.;
their diurnal variation was observed. A consistency check was performed before the inversion to
Tang, X.; Bian, J.; Yu, K.; Wang, W.
obtain a correction factor. Based on the sensitivity of geometric angles to oxygen dimer air mass
Ground-Based MAX-DOAS
factor (O4 AMF, AMF is the ratio of the slanted column density to the vertical column density), the
Measurements of Tropospheric
parameterization scheme of geometric angles in the lookup table is optimized. The results show that
Aerosols, NO2, and HCHO
Distributions in the Urban
the aerosol increased significantly in the afternoon. The diurnal variation of tropospheric NO2 and
Environment of Shanghai, China. HCHO vertical column densities (VCDs) are bimodal and unimodal patterns respectively, and their
Remote Sens. 2022, 14, 1726. https:// values are higher than those of GOME-2 and OMI satellite products. A process of aerosol reduction
doi.org/10.3390/rs14071726 and recovery are related to ground particulates and meteorological elements. The chemical sensitivity
of local ozone production also has a clear diurnal variation.
Academic Editor: Daniele Bortoli

Received: 10 December 2021 Keywords: multi-axis; differential optical absorption spectroscopy; lookup table; aerosol extinction
Accepted: 28 March 2022 coefficient profile; tropospheric vertical column densities
Published: 3 April 2022

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published maps and institutional affil- 1. Introduction
iations. At present, atmospheric pollution has become a global focus problem, which mani-
fested as the increase of primary particles, secondary particles, and trace gas. These have
a certain influence on climate and human health. The increase in soot, nitrogen oxides,
hydrocarbons, etc. in the atmosphere is related to the massive combustion of coal and oil.
Copyright: © 2022 by the authors.
Ultra Fine Particles (UFP) are respirable particles deposited efficiently in human airways
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penetrating deep within the lung and are of great importance. Urban air pollution is an im-
This article is an open access article
portant accelerating factor in the deterioration of materials in modern and cultural heritage
distributed under the terms and
buildings. The Shanghai area presents the characteristics of complex pollution with the
conditions of the Creative Commons
Attribution (CC BY) license (https://
coexistence of gaseous pollutants and particulate matter. The accumulation of aerosol and
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trace gases data is very necessary for exploring atmospheric photochemistry and pollution
4.0/).
evolution. Due to the fact that the heterogeneous chemical conversions depend on surface

Remote Sens. 2022, 14, 1726. https://doi.org/10.3390/rs14071726 https://www.mdpi.com/journal/remotesensing

Remote Sens. 2022, 14, 1726 2 of 15

and bulk concentrations, diffusion measurements in or on aerosol particles have been per-
formed using remote sensing techniques. Multi-axis differential absorption spectroscopy
(MAX-DOAS) can obtain the vertical column densities (VCDs) and vertical distribution of
aerosol and trace gases by measuring the ultraviolet/visible absorption spectrum of zenith
and multiple off-axis directions (Platt and Stutz, 2008; Irie et al., 2011) [1,2]. In addition,
as a remote sensing observation method, MAX-DOAS has the advantages of large-scale,
continuous real-time monitoring and simple structure. It can identify the types of clouds
and aerosols, and verify satellite data and chemical model data. To deeply investigate the
pollution characteristics in Shanghai, this article uses MAX-DOAS to retrieve the aerosol
profiles and the troposphere NO2 , HCHO VCDs [3–5].
In order to reduce the impact of aerosol vertical distribution to trace gas inversion,
the trace gas inversion process is usually split into two steps. That is, retrieval of aerosol
profiles firstly, and retrieval of trace gas considering the aerosol information (Wang et al.,
2013a, b) [6,7]. Wagner et al. (2011) [8] retrieved the aerosol, HCHO, and NO2 profiles of
Milan in the summer of 2003 using the lookup table. Li et al. (2010, 2013) [9,10] performed
MAX-DOAS measurements to retrieve aerosol extinction coefficient profile and the vertical
distribution of NO2 , HCHO, and CHOCHO by lookup table during the PRiDe-PRD2006
campaign in the Pearl River Delta region 50 km north of Guangzhou, China, for four
weeks in June 2006. The lookup table method is simple and can retrieve aerosol optical
depth (AOD) and boundary layer height accurately. Its inversion targets are several
parameters, which contain the profile information. Moreover, Wagner et al. (2004) [11]
proposed that they can use O4 absorption to retrieve aerosol extinctions. In addition, the
optimal estimation method is also a commonly used inversion method. Vlemmix et al.
(2015) [12] applied the lookup table method and optimal estimation method to retrieve
the tropospheric NO2 and HCHO VCDs. They found the best agreement between the two
methods for tropospheric NO2 (HCHO) VCDs and a correlation of 0.99 (0.95). However, the
two methods also have systematic bias, which is more accurate and needs to be tested by
direct detection in the future. However, Irie et al. (2012) [13] compared the tropospheric
NO2 VCDs with three satellites in six sites in East Asia to find these deviations were small.
So, the retrieval by MAX-DOAS technique is accurate and representative.
In this paper, the aerosol extinction coefficient profile of Shanghai was retrieved by a
lookup table in the summer of 2015, and then the retrieval of tropospheric NO2 and HCHO
VCDs used the two-step method. Comparing the retrieval results with satellite data was to
verify the accuracy of the inversion algorithm. A process of aerosol concentration reduction
and recovery was chosen to analyze the change reason. Finally, the diurnal variation of
chemical sensitivity of local ozone production (PO3 ) was explored. Of note, the lookup
table parameterized design scheme in this paper is based on the previous study (Li et al.,
2010; Wang, 2012) [9,14] using the results of O4 AMF sensitivity to geometric angles to
interpolate geometric angles reasonably is for improving efficiency and reducing error.

2. Analysis of Experimental Data

The multi-axis differential absorption spectrometer developed by Fudan University
was used to automatically observe Shanghai (31.29◦ N, 121.5◦ E) from July to August 2015.
The geographic location is shown in Figure 1. The spectrometer covers the spectral range
from 255 nm to 440 nm with a spectral resolution of 0.75 nm full width at half maximum. In
a measurement cycle, the elevation angle (ELE) of the telescope point to 3◦ , 6◦ , 10◦ , 18◦ , and
90◦ by turn. One cycle is about 5 min, and there are about 120 measuring cycles in a day.
Remote Sens. 2022, 14, 1726 3 of 15

Figure 1. The location of the MAX-DOAS instrument.

The measured scattered light spectra are analyzed using QDOAS software (Danckaert
T, Fayt C, Van Roozendael M, De Smedt I, Letocart V, Merlaud A, Pinardi G.; Version
2.109; Royal Belgian Institute for Space Aeronomy (BIRA-IASB);Uccle, Belgium; 9 April
2015) to retrieve the differential slant column density (DSCD). The concentration of a
given absorber integrated along the effective light path is relative to the amount of the
same absorber in a measured reference spectrum (DSCD = SCD-SCDref) of O4 , NO2 ,
and HCHO. In order to remove the Fraunhofer lines in the solar spectrum, the reference
spectrum chose the measured spectrum at solar zenith angle (SZA) = 13.2◦ at 12:00 LT
(local time, LT = UTC + 8 h) on 4 August 2015. The following O4 , NO2, HCHO DSCDs
were determined by a DOAS fit in the wavelength range 337~370 nm, 411~435 nm, and
336~359 nm, respectively. Table 1 gives cross-sections used in DOAS fitting, and the
absorption structure of Ring effect is calculated using QDOAS software in advance. In this
paper, we only considered the data with high signal noise ratio (SNR), which refers to the
DSCD data whose ratio of the obtained DSCD deviation by inversion to the DSCD is less
than 0.2. Only data with root mean square (RMS) less than 1 × 10−4 were used. Based on
the above criteria, 10% of the original data were removed.
Remote Sens. 2022, 14, 1726 4 of 15

Table 1. The parameters of cross-sections and Ring effect in QDOAS.

Species Cross Section Temperature Data Source a

O4 293 ◦ K Thalman Volkamer (2013)
HCHO 297 ◦ K Meller, MPI Mainz (1992)
BrO 223 ◦ K Fleischmann (2000)
O4
NO2 293 ◦ K Bogumil (2003)
O3 223 ◦ K Serdyuchenko (2014)
Ring - QDOAS
NO2 293 ◦ K Bogumil (2003)
O4 293 ◦ K Thalman Volkamer (2013)
NO2
O3 223 ◦ K Serdyuchenko (2014)
Ring - QDOAS
HCHO 297 ◦ K Meller, MPI Mainz (1992)
O4 293 ◦ K Thalman Volkamer (2013)
O3 223 ◦ K Serdyuchenko (2014)
HCHO O3 293 ◦ K Serdyuchenko (2014)
NO2 293 ◦ K Bogumil (2003)
BrO 223 ◦ K Fleischmann (2000)
Ring - QDOAS
a: http://satellite.mpic.de/spectral_atlas/cross_sections/, accessed on 1 December 2021.

Here, the clear sky condition was chosen as the experiment period during the entire
observation period. Meena et al. (2004) [15] propose whether the O4 DSCD changes with
the SZA show a smooth “U” feature that can be used to determine whether the weather
is clear. According to the above method, the experiment period was selected from 6:00 to
18:00 LT in 28 July–5 August 2015. However, some afternoons were eliminated.

3. Retrieval Algorithm
Figure 2 is the flow chart for retrieving the extinction profile and tropospheric NO2 and
HCHO VCD. There are three steps. First, a consistency check comparing the measured O4 DSCD
with simulated O4 DSCD on clear-sky days with low aerosol load was conducted to obtain a
correction factor. Second, a lookup table was used to retrieve the aerosol extinction coefficient
profiles. Finally, the troposphere NO2VCD and HCHO VCD were inverted by using the two-
step method. Here, the radiative transfer model SCIATRAN3.2 was used, and the temperature
and pressure profiles from 0 to 30 km in the model have been replaced with sounding data from
IGRA Shanghai (58,362) site to make the model closer to the actual situation.

3.1. Consistency Check

Figure 3 illustrates the process of consistency check. The exponential aerosol extinction
coefficient profiles calculated by MODISL2 AOD and scaling height of the tropospheric
aerosol (Qiu et al., 2005) [16] are substituted into the model to produce simulated O4 DSCD
on clear-sky days with low aerosol load. Comparing the measured and simulated O4 DSCD,
we can get a correction factor to match them.
Through the analysis of MODISL2 AOD data, we found low aerosol situation appeared
on 30 and 31 July 2015. Terra transited local at 10:15 LT on 30 July and at 11:00 LT on 31 July,
and Aqua transited local at 13:00 LT on 30 July. So, we set up half-hour before and after the
above three satellite transit times as A, B, C experiment periods in chronological order. From
the MO DISL2 AOD data, the AOD of test A, B, C is 0.465, 0.54, 0.544, respectively. Xu et al.
(2009) [17] reported that the average scaling height of the tropospheric aerosol was 2.5 km
in Shanghai from 2001 to 2005, and the growth rate was 0.046 km·a-1 from 1961 to 2005. So,
in this study, scaling height of the tropospheric aerosol is set to 2.8 km after extrapolation.
According to the good agreement between the measured and simulated O4 DSCDs at 15◦
and 30◦ elevation (Clémer et al., 2010) [18], we use 18◦ elevation for the experiment. The
consistency check results of A, B, C experiment is illustrated in Figure 4, which displays
the measured O4 DSCDs and shows they were systematically smaller than the simulated
ones because the dependence of the O4 absorption cross-section on temperature is not
Remote Sens. 2022, 14, 1726 5 of 15

very precise. The correction factor was about 1.5, namely DSCD corrected ≈ 1.5 × DSCD
uncorrected. The correction factor of 1.5 is the ratio of the simulated value to the measured
value. From now on, unless stated differently, the O4 DSCD mentioned in this paper refers
to the corrected DSCD.

Figure 2. Flow chart for the aerosol extinction coefficient profile and tropospheric NO2 and HCHO
VCD retrieval process.

Figure 3. Flow chart for the consistency check.

Figure 4. Consistency check of A, B, C test: the model simulated DSCDs, measured DSCDs, and
corrected DSCDs at 18◦ ELE. The red lines refer to the O4 DSCDs simulated by the SCIATRAN model,
the blue lines represent the O4 DSCDs measured by the MAX-DOAS instrument, and the black lines
are the measured O4 DSCDs multiplied by the correction factor.
Remote Sens. 2022, 14, 1726 6 of 15

3.2. Aerosol Inversion

Figure 5 is the flow diagram of retrieval aerosol optical properties using the lookup
table method. First, we assumed that aerosol particles were homogeneous in the boundary
layer, while in the free troposphere it decreases exponentially with height. This type of
aerosol profile can be described with a limited set of parameters.
(
F
τ (λ) · H z≤H
E(z, λ) = (1)
β(λ) · exp(− ξz ) z>H

where E(z,λ) is the aerosol extinction coefficient with wavelength λ at height z, H denotes
the boundary layer height, τ(λ) is Tropospheric aerosol optical depth, F is the fraction of
the τ(λ) residing in the boundary layer, β(λ) is the normalization factor, and ξ is the scaling
height for aerosol.

Figure 5. Flow diagram of aerosol optical properties retrieval using a lookup table.

The relation between E(z,λ) and τ(λ) is

15km
Z
E(z, λ)dz = τ (λ) (2)
0km

The β(λ) can be calculated by

(1 − F ) · τ ( λ )
β(λ) = (3)
− Hξ − 15km
ξ · (e −e ξ )

Based on Equations (1)–(3), the aerosol extinction coefficient profiles in different states
can be obtained by using different configurations of H, τ(λ), F, β(λ) and ξ parameters (as
shown in Table 2). Putting different profiles into the SCIATRAN model to produce O4
DAMF (DAMF is the difference between the tropospheric AMF in the off-axis direction
and zenithal directions) can set up a lookup table for the relationship between aerosol
parameters and O4 DAMF. It should be noted that relative to the version of Li et al., 2010
and 2013 [9,10], we used the geometric angle of the average time for the inversion to reduce
the computation time. Then based on the O4 AMF sensitivity experiment to geometric
angles, we interpolated the geometric angles reasonably to reduce the deviation between
the average geometric angle and the measured geometric angle.
Remote Sens. 2022, 14, 1726 7 of 15

Table 2. Parameters for the lookup table.

Parameter Value
0.1~1.3, interval: 0.1; 1.5~3.0, interval: 0.25;
τ
3.0~4.0, interval: 0.5
F 0.1~1.0, interval: 0.1
H (km) 0.2~1.5, interval: 0.05
Ξ (km) 5
ELE (◦ ) 3, 6, 10, 18, 90
averaging the measured values and
SZA (◦ ) and RAA (◦ )
interpolating

Figure 6 shows the variation and slope of O4 AMF with SZA at RAA = 90◦ and with
RAA at SZA = 45◦ . For other angles, they have the same change trend and were not shown
here. It can be seen from the figure that (1) the variation trend of off-axis direction and
zenith direction is roughly the same, but the slope is different, so they need to be considered
separately; (2) The slope of O4 AMF changes with SZA is one magnitude greater than RAA,
so the interpolation scheme mainly considers the influence of SZA. The range of observation
SZA from the MAX-DOAS instrument is from 10◦ to 80◦ . According to the result of the
geometric angle sensitivity experiment, for the off-axis direction, we interpolated one time
in average geometric angle when SZA is 40◦ ~60◦ , and interpolated two times when it is
60◦ or more. For the zenith direction, it was interpolated one time every two times.

Figure 6. The variation and slope of O4 AMF with SZA when RAA = 90◦ (left), and the variation and
slope of O4 AMF with RAA when SZA = 45◦ (right). The slope graph indicates the slope of the O4
AMF change with SZA (left) and RAA (right), where the red lines refer to the off-axis direction and
the blue lines indicate the zenith direction.

The measuredO4 DAMF in Figure 5 can be calculated by measured O4 DSCD and

VCD. The VCD was 1.2 × 1043 melc 2·cm − 5. VCD can be calculated using temperature
and pressure profiles from sounding data of IGRA Shanghai (58,362) site. The smallest
χ2 using Equation (4) with a particular DAMFmodel (α) configuration can retrieve the
aerosol extinction coefficient profile. In order to reduce atmospheric fluctuations and
noise disturbances from single measurement, the DAMFmeas (α) was used in Equation (4),
Remote Sens. 2022, 14, 1726 8 of 15

which is the hourly average of measured O4 DAMF. σ ( DAMFmeas (α)) represents the
standard deviation of the DAMF measured value, and DAMFmodel (α) represents the
DAMF simulated value.

18◦ 2
DAMFmeas (α) − DAMFmodel (α)
χ (τ, F, H ) = ∑ (
2
) (4)
α =3◦
σ( DAMFmeas (α))

3.3. Trace Gas Inversion (NO2 and HCHO)

First, we define the tropospheric differential slant column densities (dSCD), which
is the difference in slant column densities between off-axis direction and zenith direction.
Then we assumed that the light path from the off-axis direction and the zenith direction is
the same in the stratosphere, SCDstrat (α) = SCDstrat (90◦ ), but the light path of the off-axis
direction in the troposphere is much longer than the zenith direction. So, the tropospheric
information can be approximated by subtracting the zenith direction information from the
off-axis direction information.

dSCD= SCD (α) − SCD (90◦ ) = ( DSCD (α) + SCDre f ) − ( DSCD (90◦ ) + SCDre f )
(5)
= DSCD (α) − DSCD (90◦ )

dSCD = SCD (α) − SCD (90◦ )

= SCDtrop (α) + SCDstrat (α) − SCDtrop (90◦ ) − SCDstrat (90◦ )
= SCDtrop (α) − SCDtrop (90◦ ) (6)
= VCDtrop · AMFtrop (α) − VCDtrop · AMFtrop (90◦ )
= VCDtrop · ( AMFtrop (α) − AMFtrop (90◦ ))
DCSD (α) − DCSD (90◦ )
VCDtrop = (7)
AMFtrop (α) − AMFtrop (90◦ )

4. Data Analysis
4.1. Aerosol
Figure 7 shows the diurnal variation of the aerosol profiles in Shanghai from 28 July to
5 August 2015. We inverted O4 DSCD in the wavelength range of MAX-DOAS, and then we
inverted the 550 nm extinction coefficient using O4 DSCD in the radiative transfer model.
Since the aerosol particles were mainly concentrated in the lower troposphere, we discuss
the aerosol situation at 0~4 km, here. It can be seen that aerosol particles were mainly
distributed on the boundary layer, and the diurnal variation of aerosol was clear. The
aerosol content is low and mainly concentrated in the low layer in the morning, increasing
gradually. The aerosol content of the whole layer was increased in the afternoon, and then
gradually decreased. Within these nine days, the aerosol content was low on 30 and 31 July,
and the aerosol content was high on 28–29 July and 1 August. At 15:00 on 29 July and
at 13:00 on 1 August, the extinction coefficient content of low-level aerosols reached the
maximum value of 2.0 km−1 in the nine days.

4.2. AOD and Boundary Layer Height

Figure 8 demonstrates the diurnal variation of the nine-day mean tropospheric AOD
and boundary layer height. According to formula (1), when the aerosol extinction profile is
obtained by the lookup table method, the AOD and boundary layer height can be obtained
by inversion. The lowest value of AOD was happed at 6:00 LT, and AOD showed a little
peak value at around early morning before 9:00 LT. AOD increased from the morning to the
afternoon gradually, reaching the 2.0 maximum value at 13:00~14:00 LT, and then decreased
with a rising at 17:00~18:00 LT. The highest AOD in the afternoon was due to the heating
condition of solar energy being strongest at that time. The temperature of near-surface
atmosphere rising can result in unstable convection and turbulent vertical transport. The
two submaximal peaks appearing at 8:00~9:00 LT and 17:00~18:00 LT were matched with
morning-evening rush hours. This shows that the influence of the coupling feedback of
Remote Sens. 2022, 14, 1726 9 of 15

polluted gas-radiation-thermodynamics-dynamic-troposphere circulation on the secondary

aerosol particles. The height of the boundary layer also had a distinct characteristic of daily
change. It increased in the morning with radiation intensity and temperature augmentation
and reached the maximum at noon. It then decreased with the decrease of the solar altitude
and the temperature.

Figure 7. Time series of aerosol extinction coefficient profiles (1~4 km) at 550 nm retrieved from MAX
DOAS measurement in Shanghai from 28 July to 5 August 2015 (6:00~18:00 LT).

Figure 8. Diurnal variation of AOD and boundary layer height in Shanghai from 28 July to
5 August 2015 (6:00~18:00 LT). The red dots indicate the tropospheric AOD, and boundary layer
height retrieved by MAX-DOAS through the lookup table method.

4.3. Tropospheric NO2 and HCHO Vertical Column Densities

The retrieved tropospheric NO2 and HCHO vertical column densities in Shanghai from
28 July to 5 August 2015 are displayed in Figure 9. The NO2 diurnal variation pattern had its
valley value at around noon, namely concave feature. The NO2 minimum value was caused
by its photolysis rate reaching the maximum at noon due to strong solar radiation. The high
value of tropospheric NO2 VCDs matched with traffic peaks, and 1 and 2 August is the
weekend, but the weekend effect is not obvious. The tropospheric HCHOVCDs increased
volatility in the morning and decreased in the afternoon showing a weak convex feature.
Remote Sens. 2022, 14, 1726 10 of 15

Figure 9. Time series of tropospheric vertical column densities of NO2 and HCHO retrieved from
MAXDOAS measurement in Shanghai from 28 July to 5 August 2015(6:00~18:00 LT).

4.4. Comparision to Satellite Products

In order to verify the accuracy of the MAX-DOAS technique inversion, we compared
the retrieved tropospheric NO2 and HCHO VCD with GOME-2 and OMI satellite products.
Here, the seven tropospheric NO2 VCD satellite products were used, namely GOME-
2/MetOp-A/NASA, GOME-2/MetOp-B/NASA, GOME-2/MetOp-A/TEMIS, GOME-
2/MetOp-B/TEMIS, OMIL2/NASA, OMIL2ovp/NASA, and OMI/TEMIS. Three kinds
of tropospheric HCHO VCD satellite products were applied, which are GOME-2/MetOp-
A/NASA, GOME-2/MetOp-B/NASA, and OMIL2/NASA.
In Figure 10, the comparison of retrieved NO2 (a) and HCHO(b) with satellite products
are shown. As can be seen, the retrieved results are significantly higher than satellite
products. The multiple of retrieved NO2 (HCHO) and corresponding satellite products is
1~5 (1~3), and the average multiple is 2.37 (1.57). The results of Li et al. 2013 show that the
NO2 VCD measured by OMI is about 20% to 50% higher than the NO2 VCD inverted by
MAX-DOAS. Previous studies have shown that the NO2 VCD measured by OMI is about
10% to 50% lower than that of ground-based measurements. Combined with our research, it
is shown that the VCD content is related to the distribution of pollutants at the observation
site. In the paper, the reason for the retrieved results being on the high side may be that the
experimental site is located in a heavily traffic-contaminated area in Shanghai, since spatial
resolution of the satellite product is low. The area contained the range of 50 km centered
on the experimental site, which not only include heavily polluted areas, but also involve
Remote Sens. 2022, 14, 1726 11 of 15

low pollution areas. Moreover, the unconsidered trace gas would influence the accuracy of
retrieval results, which is too high during the spectral data analysis process by QDOAS.

Figure 10. Comparison of concentrations of (a) NO2 and (b) HCHO tropospheric vertical column
densities retrieved by MAX-DOAS technique with satellite products. The black dots represent the
tropospheric NO2 and HCHO VCDs retrieved by DOAS, the blue dots represent the tropospheric NO2
and HCHO VCDs from the satellite products, and the red dots represent the ratio of the tropospheric
VCDs retrieved by DOAS to the tropospheric VCDs from the satellite products.

Figure 11 shows that the linear correlation between satellite products and retrieved
results. Among them, there were three satellite products having a positive correlation
with the retrieved NO2 , as shown in Figure 11a–c, while the retrieved HCHO and all its
satellite products were a linear positive correlation, as seen in Figure 11d–f. The correlation
coefficients between retrieved NO2 tropospheric VCDs and satellite products of GOME-
2/MetOp-B/NASA, GOME-2/MetOp-B/TEMIS, and OMI/TEMIS were 0.5172, 0.8449 and
0.5223, respectively. The correlation coefficients between retrieved HCHO tropospheric
VCDs and satellite products of GOME-2/MetOp-A/NASA, GOME-2/MetOp-B/NASA,
and OMI/NASA were 0.8632, 0.8896, and 0.3453, respectively. Because the samples of each
satellite product are different in the correlation analysis process, it is impossible to tell
which satellite product is closer to the retrieved result.
Remote Sens. 2022, 14, 1726 12 of 15

Figure 11. Correlation analysis of NO2 tropospheric VCD satellite products from (a) GOME-2/MetOp-
B/NASA; (b) GOME-2/MetOp-B/TEMIS; (c) OMI/TEMIS and retrieved results, Correlation analysis
of HCHO tropospheric VCD satellite products from (d) GOME-2/MetOp-A/NASA; (e) GOME-
2/MetOp-B/NASA; (f) OMIL2/NASA and retrieved results (unit: 1015 molec·cm−2 ).

4.5. A Cause Analysis of Aerosol Reduced and Recovered Process

A process that aerosol content reduced firstly and then recovered from 29 July to
1 August is shown in Figure 7. In general, local aerosol content is related to near-surface
particulate matter concentrations and meteorological elements (wind is the main factor).
The local atmospheric stability also can affect the accumulation of pollutants when chemical
factors were not considered. We obtained PM air quality monitoring data from Hongkou
Environmental Monitoring Station (3.5 km from the observation point), and meteorological
element data from Weather Ground Meteorological Company and IGRA sounding data.
The effects of aerosol were explored from the near-surface particulate concentration, wind
direction and speed, and inversion layer, as shown in Figure 12.
Figure 12a is the diurnal variation of near-surface PM10 and PM2.5 in Shanghai
from 29 July to 1 August. We can see that the PM10 and PM2.5 concentrations were low
on 30 and 31 July and then recovered on 1 August. So, comparing with the aerosol situation
in Figure 7, the PM10 and PM2.5 concentrations matched with aerosol content, indicating
the higher the particulate matter concentration, the higher the aerosol content. Figure 12b
is the diurnal variation of wind direction and wind speed in this process. From 29 July to
30 July, low aerosol content is shown when winds mainly blew from the east and southeast,
because the cleaner air came from the south and southeast sides of Shanghai. On 1 August,
high aerosol was prominent with southwest and west wind because heavy pollution area
is situated to the southwest of the observation site.
Remote Sens. 2022, 14, 1726 13 of 15

Figure 12. Diurnal variation of (a) PM10 and PM2.5, (b) wind direction and wind speed in Shanghai
from 28 July to 5 August 2015, and (c) Inversion layer at 20:00 on 29 July, 30 July, and 1 August.

Figure 12c shows the inversion layer occurred during this process. There are inversion
layers below 60 m at 20:00 LT on 29 July and 30 July, which inversion intensities were 0.656
and 0.345, respectively. There was no inversion layer on 31 July, and an inversion layer
whose inversion intensity was 0.687 appeared at 420 m to 680 m at 20:00 LT on 1 August.
So, the inversion layer was related to the aerosol content, that aerosol content decreased
(increased) when the inversion layer weakened (enhanced), by analyzing the relationship
between the inversion layer with this aerosol process.

4.6. Study on Chemical Sensitivity of Local Ozone Production

We used the ratio of tropospheric HCHO and NO2 VCDs to explore the chemical
sensitivity of local ozone production (PO3 ). The ratio was less than 1, which indicates
this area was at a VOCs-limited condition. When the ratio is between 1 and 2, the PO3
was at a mixed VOC-NOx-limited regime. The ratio was larger than 2 with NOx -limited
condition of PO3 (Duncan et al., 2005) [19]. Figure 13 shows the ratio which indicated
the PO3 in Shanghai during nine days. The ratio of tropospheric HCHO and NO2 VCDs
had a daily change during the experiment period. The ratio was near one with a slight
decrease from 6:00 LT to 10:00 LT. The ratio from 10:00 to 13:00 increased significantly and
the maximum value can reach three, and then gradually decreased after 13:00. During the
nine-day experimental period, PO3 in one day can be summarized as follows: VOCs-limited
Remote Sens. 2022, 14, 1726 14 of 15

condition–mixed VOC-NOx-limited regime—NOx -limited condition—mixed VOC-NOx -

limited regime—VOCs-limited condition. This diurnal variation pattern of PO3 correlated
with the daily change of HCHO, NO2 tropospheric VCDs.

Figure 13. The ratio of tropospheric HCHO and NO2 vertical column densities in Shanghai from
28 July to 5 August 2015 (6:00~18:00 LT).

5. Conclusions
Aerosol extinction profiles at 550 nm were retrieved using multi-axis differential
optical absorption spectroscopy and a lookup table/. Then the tropospheric NO2 and
HCHO vertical column densities were retrieved by applying a two-step method from
28 July 2015 to 5 August 2015 in Shanghai. The results show that the aerosol in summer in
Shanghai will increase in the afternoon, and the tropospheric NO2 and HCHO VCD have
concave and convex structures, respectively. The retrieved tropospheric NO2 and HCHO
VCDs are significantly higher than satellite products. Wind direction and inversion layer
can influence the aerosol pollution process. PO3 has an obvious diurnal variation during
the experimental period.
The lookup table used in this paper can retrieve the aerosol extinction coefficient
profile accurately. The O4 AMF sensitivity experiment to the geometric angle can be used
to optimize the geometrical angle configuration in the lookup table. However, the aerosol
profile shape setting is too single and needs further optimization.

Author Contributions: Conceptualization, K.Y. and W.W. (Weiguo Wang); methodology, W.W.
(Wanlin Wei); software, K.Y.; validation, K.Y., H.W. and W.W. (Wanlin Wei); formal analysis, H.C.;
investigation, J.B.; resources, K.Y.; data curation, X.T. and H.W.; writing—original draft, X.T.; prepara-
tion, K.Y.; writing—review and editing, W.W. (Wanlin Wei); visualization, H.W.; supervision, K.Y.;
project administration, H.W.; funding acquisition, All authors have read and agreed to the published
version of the manuscript.
Funding: This research was funded by [Second Tibetan Plateau Scientific Expedition and Research
Program (STEP)] grant number [2019QZKK0604]; funded by [National Science Fund for Distinguished
Young Scholars and the National Natural Science Foundation of China] grant number [41825011,
41807308, 21777026, 41641044, and 21477021]; funded by [Open Project of Shanghai Key Laboratory
of Atmospheric Particle Pollution and Prevention (LAP3)] grant number [FDLAP19009].
Institutional Review Board Statement: “Not applicable” for studies not involving humans or animals.
Informed Consent Statement: Informed consent was obtained from all subjects involved in the study.
Data Availability Statement: The data are not publicly available due to the data will be used in
future studies.
Acknowledgments: Thanks to the observations data of the MAX-DOAS instrument provided by
Fudan University. The QDOAS software we used for DOAS analysis is provided by the Belgian
Institute for Space and Aeronomy (IASB/BIRA). Furthermore, we would like to thank the Institute
of Environmental Physics (IUP) and Remote Sensing (IFE) at Bremen University, which provide
the SCIATRAN model. We also acknowledge the free use of tropospheric NO2 and HCHO column
data from NASA and TEMIS. This work was supported by the “Second Tibetan Plateau Scientific
Remote Sens. 2022, 14, 1726 15 of 15

Expedition and Research Program (STEP)” (grant no. 2019QZKK0604), the National Science Fund
for Distinguished Young Scholars and the National Natural Science Foundation of China (grant
nos. 41825011, 41807308, 21777026, 41641044, and 21477021), and the Open Project of Shanghai Key
Laboratory of Atmospheric Particle Pollution and Prevention (LAP3) (grant no. FDLAP19009).
Conflicts of Interest: The authors declare no conflict of interest.

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