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**Atmospheric Chemistry and Physics**
An interactive open-access journal of the European Geosciences Union

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- About
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**Research article**
28 Jan 2019

**Research article** | 28 Jan 2019

Effects of turbulence structure and urbanization on the heavy haze pollution process

^{1}Laboratory for Climate and Ocean-Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing 100081, P.R. China^{2}State Key Laboratory of Severe Weather, Chinese Academy of Meteorological Sciences, Beijing 100081, P.R. China^{3}Tianjin Municipal Meteorological Bureau, Tianjin 300074, P.R. China^{4}State Key Joint Laboratory of Environmental Simulation and Pollution Control, Department of Environmental Science, Peking University, Beijing 100081, P.R. China

^{1}Laboratory for Climate and Ocean-Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing 100081, P.R. China^{2}State Key Laboratory of Severe Weather, Chinese Academy of Meteorological Sciences, Beijing 100081, P.R. China^{3}Tianjin Municipal Meteorological Bureau, Tianjin 300074, P.R. China^{4}State Key Joint Laboratory of Environmental Simulation and Pollution Control, Department of Environmental Science, Peking University, Beijing 100081, P.R. China

**Correspondence**: Hongsheng Zhang (hsdq@pku.edu.cn)

**Correspondence**: Hongsheng Zhang (hsdq@pku.edu.cn)

Abstract

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In this paper, an automated algorithm is developed, which is used to identify the spectral gap during the heavy haze pollution process, reconstruct acquired data, and obtain pure turbulence data. Comparisons of the reconstructed turbulent flux and eddy covariance (EC) flux show that there are overestimations regarding the exchange between the surface and the atmosphere during heavy haze pollution episodes. After reconstruction via the automated algorithm, pure turbulence data can be obtained. We introduce a definition to characterize the local intermittent strength of turbulence (LIST). The trend in the LIST during pollution episodes shows that when pollution is more intense, the LIST is smaller, and intermittency is stronger; when pollution is weaker, the LIST is larger, and intermittency is weaker. At the same time, the LIST at the city site is greater than at the suburban site, which means that intermittency over the complex city area is weaker than over the flat terrain area. Urbanization seems to reduce intermittency during heavy haze pollution episodes, which means that urbanization reduces the degree of weakening in turbulent exchange during pollution episodes. This result is confirmed by comparing the average diurnal variations in turbulent fluxes at urban and suburban sites during polluted and clean periods. The sensible heat flux, latent heat flux, momentum flux, and turbulent kinetic energy (TKE) in urban and suburban areas are all affected when pollution occurs. Material and energy exchanges between the surface and the atmosphere are inhibited. Moreover, the impact of the pollution process on suburban areas is much greater than on urban areas. The turbulent effects caused by urbanization seem to help reduce the consequences of pollution under the same weather and pollution source condition, because the turbulence intermittency is weaker, and the reduction in turbulence exchange is smaller over the urban underlying surface.

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Ren, Y., Zhang, H., Wei, W., Wu, B., Cai, X., and Song, Y.: Effects of turbulence structure and urbanization on the heavy haze pollution process, Atmos. Chem. Phys., 19, 1041–1057, https://doi.org/10.5194/acp-19-1041-2019, 2019.

1 Introduction

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PM_{2.5} (fine particular matter, with a diameter smaller than
2.5 µm) has become the foremost pollution issue in China (Zhang et
al., 2012; Hu et al., 2014), particularly in Beijing and its vicinity, in
terms of severity and duration (Watts, 2005; Tang et al., 2009, 2012, 2015;
Zhang et al., 2014; Yang et al., 2015). Because of its negative impacts on
human health (Dominici et al., 2014; Thompson et al., 2014) and complicated
effects on weather and climate (Liepert et al., 2004; Wang et al., 2010,
2015a, b; Q. Zhang et al., 2015), heavy aerosol pollution has prompted the close attention of
not only scientists but also the government and ordinary people.

During pollution periods, previous studies have indicated that meteorological
conditions always include constant stagnant winds, relatively increased
water-vapour density, and strong stable stratification, which inhibits the
diffusion of vertical pollution and results in the explosive growth of
PM_{2.5} in Beijing (L. Zhang et al., 2015; R. Zhang et al., 2015; Wei et al., 2018; Zhong et al.,
2018). The diurnal variations in particulate concentrations are mostly
dominated by the diurnal variability of the boundary layer and source
emissions (Liu et al., 2014); turbulent motion determines the meteorological
elements in the atmospheric boundary layer, such as turbulence diffusion, PBL
height, and atmospheric circulation patterns, are all key to hazy weather
(Wang et al., 2015a, b; Tang et al., 2016; Zhu et al., 2018; Zhang et al., 2016)
and dominate whether the haze occurs or not, since emissions can remain
stable within a defined period in a certain area. Therefore, the spatial and
temporal characteristics of turbulent activity have significant effects on
the local air quality from hourly to diurnal scales under a stable boundary
layer (Salmond and McKendry, 2005).

Turbulence in the stable boundary layer is weak and typically characterized by intermittent turbulence or even no turbulence at a variety of heights, temporal scales, and spatial locations (Mahrt, 1998, 2014; Coulter and Doran, 2002; Van de Wiel et al., 2003; Salmond, 2005). The term intermittency has different meanings that vary among studies (Coulter and Doran, 2002; Muschinski et al., 2004; Acevedo et al., 2006; Mahrt, 2007a). Mahrt (1989, 1999) defines intermittency as the case where eddies at all scales are missing or suppressed at scales that are large compared to those for large eddies. A number of studies have indicated that intermittency is driven by nonstationarity due to motion on timescales that are slightly greater than those for turbulence (Mahrt, 2007a, 2010b) when the large-scale flow is weak. These motions are sometimes referred to as submesoscale motions (Nappo, 2002; Sun et al., 2004; Anfossi et al., 2005; Conangla et al., 2008; Mahrt et al., 2008). Some studies have simply defined intermittency as “another name for nonstationary” (Treviño, 2000).

As mentioned earlier, the occurrence of heavy haze is always accompanied by low wind speeds and strong stable stratification. Under these conditions, exchanges between the surface and the atmosphere cannot be calculated with the eddy-correlation technique when intermittent turbulence exists because of the nonstationarity imposed by submesoscale motions (Vickers and Mahrt, 2006; Acevedo et al., 2006, 2007; Aubinet, 2008; Mahrt, 2010a), which makes it very difficult to accurately determine the transport, storage, and diffusion of pollutants, particularly in regions with complex terrain (Bowen et al., 2000), such as Beijing. Densely constructed buildings on the underlying surface aggravate the complexity of turbulent exchange during pollution periods, and the impact of urbanization on pollution is unknown. The Monin–Obukhov similarity theory establishes the relationship between turbulent flux and the vertical gradient in the surface layer and has been widely used in weather and climate models (Wood et al., 2010; Wilson, 2008). However, turbulent flux calculated by the traditional time-averaging method is contaminated by submesoscale motions during the heavy pollution process, which makes the application of similar theories difficult and may be the reason that the simulated pollutant concentration is lower during the heavy pollution process (Li et al., 2016). To provide a basis for improving the parameterization scheme of the atmospheric pollution diffusion model, it is very important to accurately calculate pure turbulent transport during the heavy pollution process.

Therefore, the purpose of this study is to separate classic turbulent motions from submesoscale motions. At the same time, intermittency can be defined by the turbulent and nonturbulent portions of a signal once the criteria for identifying the boundary between them have been established (Salmond, 2005). Only in this way can we identify the classic turbulence exchange during pollution periods, regardless of whether turbulence occurs over a flat underlying surface or a complex underlying surface. In a previous study, Muschinski (2004) found a plateau in the intermittency spectra. Vickers and Mahrt (2003) showed the existence of a cospectral gap, which separated turbulent and mesoscale contributions to calculate the fluxes in heat, moisture, and momentum using the multiresolution decomposition technique. Salmond (2005) used the wavelet analysis to objectively isolate intermittent turbulent bursts within vertical velocity time series. Wei et al. (2017) found that the spectral gap separates fine-scale turbulence from large-scale motions using the arbitrary-order Hilbert spectral analysis during intermittency in the Cooperative Atmosphere–Surface Exchange Study-1999 (CASE-99). Because of the nonstationarity and nonlinearity of intermittent turbulence, analytical techniques have significant impacts on the results. A new technique, named the arbitrary-order Hilbert spectral analysis (Huang et al., 2011), showed its advantage and validity in the application of turbulent flow and intermittency (Wei et al., 2016, 2017, 2018).

In this paper, we use the arbitrary-order Hilbert spectral method to analyse
turbulence data observed during several severe haze pollution episodes that
occurred in Beijing and its nearby suburbs from 16 December 2016 to
8 January 2017 to identify the spectral gap and separate classic turbulence
from the original signal. After obtaining the pure turbulence signal and the
strength of the submesoscale motions, the classic turbulent flux and
intermittency strength can be calculated. Then, we can obtain the
macrostatistical characteristics of turbulence over a flat terrain in
suburban Beijing and discover the difference between clean and polluted days.
This analysis is helpful for improving the current understanding of the
transport and diffusion of PM_{2.5} and the intermittency strength of
turbulence when heavy haze pollution occurs. The effect of urbanization on
the heavy pollution process is simultaneously studied by comparing the
results of the urban and suburban sites.

2 Description of the sites and data

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The data used in this paper are from two measurement sites (Fig. 1 shows the
location of the two sites). Data over a flat terrain were collected at a
continuous measurement site (40.16^{∘} N, 116.28^{∘} E) in a
Beijing suburb. The observational site was set up in the middle of a vast and
horizontal farmland, near the Changping county. A 10 m tower was erected for
the eddy covariance (EC) and meteorological measurements. The EC system was
mounted at a height of 8.3 m above ground, which was located within the
surface layer. The system was equipped with an integrated
CO_{2}–H_{2}O open-path gas analyzer and three-dimensional
sonic anemometer-thermometer (IRGASON, Campbell Scientific, Inc., USA). The
IRGASON was levelled and pointed north. The turbulence data, such as the
horizontal wind vector, virtual temperature, and water vapour content, were
collected using a data logger (CR3000, Campbell Scientific, Inc., USA) at a
frequency of 10 Hz and were averaged over an interval of 30 min for the
analysis of meteorological elements. For convenience of description, this
site is described as the suburban site.

The second data set was collected over urban terrain at a continuous
measurement site at Peking University (39.99^{∘} N, 116.31^{∘} E) in Beijing, which is the capital of China. The instruments are situated
on top of a building at the School of Physics (Peking University) and extend
25 m above ground. There are teaching and residential buildings and public
transit facilities that surround the station. The site is located in a
typical urban landscape. The buildings around the site are neat and uniform,
and the average building height is 20 m. So observations at the urban site are
located within the surface layer. Details on the site introduction and data
background have been shown in Ren et al. (2018). The concentrations of
PM_{2.5} were collected using a Thermo Fisher Scientific instrument (series
FH-62-C14), and 30 min averaging time series were performed to remove
outliers. The system was equipped with an integrated CO_{2}∕H_{2}O open-path gas
analyzer (LI-7500, LI-COR Biosciences, Inc., USA) and three-dimensional
sonic anemometer-thermometer (IRGASON, Campbell Scientific, Inc., USA). The
IRGASON was levelled and pointed north. The turbulence data such as the
horizontal wind vector, virtual temperature, and water vapour content were
collected using a data logger (CR3000, Campbell Scientific, Inc., USA) at a
frequency of 10 Hz and were averaged over an interval of 30 min for the
analysis of meteorological elements. For convenience of description, this
site is described as the urban site.

The suburban site is 20 km away from the urban site. At this distance, the
large-scale weather background is consistent. Because of the flat terrain of the
suburban site, it was used as a reference. The sources of PM_{2.5} of
the two sites are generally consistent. The observations of PM_{2.5} at urban
sites are used to represent the evolution of the entire pollution process,
as this study focuses on pollution processes rather than specific values.
Since the observations at both sites are located in the surface layer, i.e.,
the constant flux layer, the values of turbulence flux are comparable.

In this study, we select a 24-day pollution period from 16 December 2016 to
8 January 2017; the number of heavy pollution days with PM_{2.5}
concentrations exceeding 200 µg m^{−3} reached 15 (17–21, 24–25, 28,
and 30–31 December 2016 and 1–7 January 2017). The remaining days were
identified as clear days. The PM_{2.5} mass concentration, horizontal wind
speed, virtual temperature, and water vapour mixing ratio are shown in Fig. 2
for the days of concern. The trends in meteorological elements over time
are consistent at both sites. The horizontal wind speed is larger during
clear days and smaller during pollution days; the virtual temperature seems
to be greater during pollution days, but this result is not obvious. The
water-vapour content is significantly higher during pollution days than
during clear days. The characteristics of these meteorological elements
during the pollution process are similar to those in previous studies (Wang
et al., 2014; Sun et al., 2014; Tai et al., 2010).

The raw turbulence data were preprocessed over an averaging interval of
30 min by the Eddy Pro software (Advanced 4.2.1, LI-COR Biosciences, Inc.,
USA). Preprocessing included procedures involving error flags, despiking
(following Vickers and Mahrt, 1997), double rotations (following Wilczak et
al., 2001), and detrending, which are implemented using the block-averaging
method. In this paper, the EC method is used to calculate the flux for
comparison, where the average time is 30 min. At the same time, strict
quality control is performed on the data and data groups to remove data
meeting any of the following conditions: (1) the EC method runs with more
than $\pm \mathrm{120}{}^{\circ}$ between the wind direction and direction of the sonic
anemometer, (2) the included angle between the wind direction and horizontal
plane is greater than 3^{∘}, (3) the wind speed is less than
0.5 m s^{−1}, (4) the friction speed is less than 0.05 m s^{−1},
(5) the sensible heat flux is less than 5 W m^{−2}, and (6) data groups
are obviously incorrect.

3 Methodology

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The physical quantities used in this paper are turbulent kinetic energy
(TKE), several variances (*σ*_{u}, *σ*_{v}, *σ*_{w}, *σ*_{θ}, and *σ*_{q}),
friction speed (*u*_{∗}), and fluxes ($-\stackrel{\mathrm{\u203e}}{{u}^{\prime}{w}^{\prime}}$,
$\stackrel{\mathrm{\u203e}}{{w}^{\prime}{\mathit{\theta}}^{\prime}}$ and $\stackrel{\mathrm{\u203e}}{{w}^{\prime}{q}^{\prime}}$). Among these, the TKE is
calculated as

$$\begin{array}{}\text{(1)}& e={\displaystyle \frac{\mathrm{1}}{\mathrm{2}}}\left(\stackrel{\mathrm{\u203e}}{{{u}^{\prime}}^{\mathrm{2}}}+\stackrel{\mathrm{\u203e}}{{{v}^{\prime}}^{\mathrm{2}}}+\stackrel{\mathrm{\u203e}}{{{w}^{\prime}}^{\mathrm{2}}}\right),\end{array}$$

the variance is calculated as

$$\begin{array}{ll}{\displaystyle}& {\displaystyle}{\mathit{\sigma}}_{u}=\stackrel{\mathrm{\u203e}}{{u}^{\prime}{u}^{\prime}},\\ {\displaystyle}& {\displaystyle}{\mathit{\sigma}}_{v}=\stackrel{\mathrm{\u203e}}{{v}^{\prime}{v}^{\prime}},\\ {\displaystyle}& {\displaystyle}{\mathit{\sigma}}_{w}=\stackrel{\mathrm{\u203e}}{{w}^{\prime}{w}^{\prime}},\\ {\displaystyle}& {\displaystyle}{\mathit{\sigma}}_{\mathit{\theta}}=\stackrel{\mathrm{\u203e}}{{\mathit{\theta}}^{\prime}{\mathit{\theta}}^{\prime}},\\ \text{(2)}& {\displaystyle}& {\displaystyle}{\mathit{\sigma}}_{q}=\stackrel{\mathrm{\u203e}}{{q}^{\prime}{q}^{\prime}},\end{array}$$

the turbulence flux is calculated as

$$\begin{array}{ll}{\displaystyle}& {\displaystyle}\mathit{\tau}=\mathit{\rho}{u}_{\ast}^{\mathrm{2}}=\mathit{\rho}\stackrel{\mathrm{\u203e}}{{u}^{\prime}{w}^{\prime}},\\ {\displaystyle}& {\displaystyle}H=\mathit{\rho}{C}_{p}\stackrel{\mathrm{\u203e}}{{w}^{\prime}{\mathit{\theta}}^{\prime}},\\ \text{(3)}& {\displaystyle}& {\displaystyle}E=\mathit{\rho}\stackrel{\mathrm{\u203e}}{{w}^{\prime}{q}^{\prime}}\end{array}$$

and the friction speed is calculated as

$$\begin{array}{}\text{(4)}& {u}_{\ast}={\left[{\left(-\stackrel{\mathrm{\u203e}}{{u}^{\prime}{w}^{\prime}}\right)}^{\mathrm{2}}+{\left(-\stackrel{\mathrm{\u203e}}{{v}^{\prime}{w}^{\prime}}\right)}^{\mathrm{2}}\right]}^{{\scriptscriptstyle \frac{\mathrm{1}}{\mathrm{4}}}}.\end{array}$$

In the traditional turbulence theory, Van der Hoven (1957) presented an
analysis on the large spectrum of horizontal wind speeds, which showed a
notable spectral gap of approximately 1 cycle h^{−1} between the
macroscale (synoptic) and microscale (turbulent) parts of the spectrum. Many
other studies have generally proven the existence of the spectral gap
(Panofsky, 1969; Fiedler and Panofsky, 1970; Smedman-Högström and
Högström, 1975). As observations progressed, many studies on the
stable boundary layer have indicated that the turbulent part of the signal
decreases, the timescale for turbulence decreases, and the timescale for
the spectral gap also decreases, as mentioned above. These studies used the
multiresolution decomposition method to choose a variable averaging time to
remove the effects of mesoscale motions. The method we used here to separate
pure turbulence and submesoscale motion is based on half-hourly data (i.e., the
fixed averaging time). The multiresolution basis utilized is a wavelet set,
as it is the only wavelet set that satisfies Reynolds averaging (Howell and
Mahrt, 1997; Mallat, 1998; Vickers and Mahrt, 2003, 2006). In this study, we
adopt the Hilbert–Huang transform (Huang et al., 1998, 1999), which is fully
data-driven and local in both the physical and frequency domains (Huang et
al., 1998; Flandrin et al., 2004). The advantages of researching turbulence
data that are nonstationary and nonlinear have been proven previously (Huang
et al., 2008, 2013; Schmitt et al., 2009; Wei et al., 2013, 2016, 2017).

The spectral gap was examined by studying the second-order Hilbert spectra
(*u*^{′}, *v*^{′}, *w*^{′}, *θ*^{′}, and
*q*^{′}) for each 30 min period. The calculation method
for the second-order Hilbert spectra comes from the arbitrary-order Hilbert
spectral analysis (Huang et al., 2008), which is an extended version of the
Hilbert–Huang transform. A joint probability density function (PDF),
*p*(*ω*, *A*), can be extracted from *ω*_{i} and
*A*_{i} for all intrinsic mode functions. Then, the arbitrary-order Hilbert
marginal spectrum is defined as an amplitude-frequency space by the marginal
integration of the joint PDF *p*(*ω*, *A*):

$$\begin{array}{}\text{(5)}& {L}_{q}\left(\mathit{\omega}\right)=\int p(\mathit{\omega},A){A}^{q}\mathrm{d}A,\end{array}$$

where *ω* represents the instantaneous frequency, *A* represents the
instantaneous amplitude, *q*≥0 represents the arbitrary moment, and
*p*(*ω*, *A*) represents the PDF. Specifically, *h*(*ω*) corresponds
to the second-order Hilbert marginal spectrum ($h\left(\mathit{\omega}\right)={L}_{\mathrm{2}}\left(\mathit{\omega}\right)=\int p(\mathit{\omega},A){A}^{\mathrm{2}}\mathrm{d}A$).

An automated algorithm was developed to objectively find the frequency
location of the spectral gap. This method is based on the characteristics in
Fig. 4b in Wei et al. (2017). The spectral gap between turbulence and the
submesoscale motions is identified as the frequency interval in which the
second-order Hilbert spectral values are approximately constant, or the slope
is approximately equal to 0. Figure 3 shows the second-order Hilbert spectra
from the newly reconstructed data and raw data. As shown in Fig. 3a, the
lower-frequency limit of the spectral gap is *ω*=0.008 Hz, and the
upper-frequency limit is not used to reconstruct the data. The part of the
frequency larger than *ω* indicates the turbulence signal, and the part
of the frequency smaller than *ω* indicates nonstationary motion, which
has a scale larger than that for turbulence. Then, we can search for the mode
of the intrinsic mode function (IMF) (*N*=9 in this case), which has the mean
frequency closest to *ω*. Therefore, modes 1–*N* are chosen to
reconstruct the pure turbulence signal, and the remaining modes are chosen to
reconstruct the signal of the submesoscale motion.

As shown in Figs. 3a–c, it is obvious that the reconstruction successfully eliminated the energy contained by large-scale motion while retaining turbulent energy. The new spectrum, which is shown by the black dotted lines in Fig. 3, is consistent with the structure of the turbulent energy spectrum in the classic theory. We reconstructed the data for all time periods when the spectral gap existed in our data set. The results of the total reconstructed data spectrum showed that the whole process removed the effects of large-scale motion and retained classic turbulence, while simultaneously obtaining large-scale motions.

We use the ratio of turbulent intensity compared to all signals to indicate the intermittent strength. To obtain the strength of submesoscale motion, we introduce the definition of the velocity scale for submesoscale motion from Mahrt (2007b, 2009, 2010b, 2011). The velocity scale for submesoscale motion represents the kinetic energy of submesoscale motions and is defined as follows:

$$\begin{array}{}\text{(6)}& {V}_{\mathrm{smeso}}=\sqrt{{{u}^{\prime}}_{\mathrm{smeso}}^{\mathrm{2}}+{{v}^{\prime}}_{\mathrm{smeso}}^{\mathrm{2}}+{{w}^{\prime}}_{\mathrm{smeso}}^{\mathrm{2}}},\end{array}$$

where ${{u}^{\prime}}_{\mathrm{smeso}}$, ${{v}^{\prime}}_{\mathrm{smeso}}$, and ${{w}^{\prime}}_{\mathrm{smeso}}$, represent the deviations reconstructed from the IMF corresponding to the submesoscale motions during each 30 min period. Similarly, the turbulent velocity scale is defined as follows:

$$\begin{array}{}\text{(7)}& {V}_{\mathrm{turb}}=\sqrt{{{u}^{\prime}}_{\mathrm{turb}}^{\mathrm{2}}+{{v}^{\prime}}_{\mathrm{turb}}^{\mathrm{2}}+{{w}^{\prime}}_{\mathrm{turb}}^{\mathrm{2}}},\end{array}$$

where ${{u}^{\prime}}_{\mathrm{turb}}$, ${{v}^{\prime}}_{\mathrm{turb}}$, and ${{w}^{\prime}}_{\mathrm{turb}}$, represent the deviations reconstructed from the IMF corresponding to the turbulent motions during each 30 min period. Then, we can define the local intermittent strength from an energy point of view as follows:

$$\begin{array}{}\text{(8)}& \mathrm{LIST}={\displaystyle \frac{{V}_{\mathrm{turb}}}{\sqrt{{V}_{\mathrm{smeso}}^{\mathrm{2}}+{V}_{\mathrm{turb}}^{\mathrm{2}}}}}.\end{array}$$

The value of the LIST is equal to the ratio of turbulent intensity in the acquired signal. When the LIST is large and close to 1, there are more turbulent components in the acquired signal, the influence of the submesoscale motion is weaker, and the intermittency is weaker. When the LIST is small and far from 1, there are fewer turbulent components in the collected signal, the influence of submesoscale motion is stronger, and the intermittency is stronger.

4 Results and discussion

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We use the automated algorithm to identify the spectral gaps in 1152 groups
of 10 Hz high-frequency data from 16 December 2016 to 8 January 2017 at the
urban and suburban sites. There are 440 groups of data in the along-wind
direction, 519 groups of data in the cross-wind direction, 390 groups of
data in the vertical direction, 467 groups of data in the scalar *θ*,
and 501 groups of data in the scalar *q*, which is where the spectral gap
occurs at the suburban site. The data sets encompassing the spectral gap
account for 38 %, 45 %, 34 %, 41 %, and 43 % of the total data at
the suburban site, respectively. The proportions are 41 % (481), 37 %
(425), 35 % (402), 41 % (476), and 45 % (520) for the *u*, *v*, *w*, *t*, and
*q* components at the urban site. The occurrence of a spectral
gap is common throughout the pollution process, which means that the effects
of nonstationary motion on the collected signals are common throughout the
process. Under these conditions, the usual half-hour length is not
suitable for stationary conditions. The eddy-correlation flux calculated
using a conventional averaging time of 30 min to define the perturbations is
severely contaminated by poorly sampled mesoscale motions.

During the half-hour period, we refer to the variance in the pure turbulent
fluctuations as the new results and that calculated via the classic EC
system is referred to as the original variance results. A comparison of the
TKE and variance parameters (*σ*_{u}, *σ*_{v}, *σ*_{w}, *σ*_{θ}, and *σ*_{q})
between the new results and original results is shown in Fig. 4, and a
comparison among the vertical heat flux ($\stackrel{\mathrm{\u203e}}{{w}^{\prime}{\mathit{\theta}}^{\prime}}$), vertical
water-vapour flux ($\stackrel{\mathrm{\u203e}}{{w}^{\prime}{q}^{\prime}}$), and momentum flux
($-\stackrel{\mathrm{\u203e}}{{u}^{\prime}{w}^{\prime}}$) is presented in Fig. 5; the fitted lines are
given in both figures. When there is no spectral gap, the 30 min time length
is suitable for stationary conditions; therefore, the classic EC method is
credible. Figures 4 and 5 only present the results when there is a
spectral gap (i.e., when there is nonstationarity at the suburban site).

All of the fitted results show that there are certain degrees of
overestimated variance in Fig. 4. The slope of the fitted line is 0.81 for
the TKE, as Fig. 4f shows, which means that the TKE originally calculated by
the conventional method is overestimated by approximately 19 %. The
comparison of *σ*_{u} and *σ*_{v} shows the
same pattern as that for the TKE. The traditional method for the half-hourly
eddy correlation overestimates by approximately 27 % (slope of 0.73) and
21 % (slope of 0.79) for *σ*_{u} and *σ*_{v},
respectively. The overestimation of *σ*_{w} is not as obvious as those
for *σ*_{u} and *σ*_{v}. The slope of the fitted
line in Fig. 4c is 0.99, which indicates that the appearance of the
spectral gap has fewer effects on the variance in vertical velocity. The
overestimation is even more pronounced when the TKE and *σ*_{u},
*σ*_{v}, and *σ*_{w} are small, which indicates that the
overestimation can be more significant when the turbulence is weak.
Similarly, we examine the variance in potential temperature and moisture
content in Fig. 4d and e. The variations in potential
temperature and moisture content are also overestimated: the difference is
that the overestimation percentages are larger. The slopes of the fitted
lines in Fig. 4d and e are 0.60 and 0.54, which means that
the traditional method for the half-hourly eddy correlation overestimates
approximately 40 % and 46 % of *σ*_{θ} and
*σ*_{q} when the spectral gap occurs. Such a
substantial overestimation cannot be ignored. In general, the
variations in *σ*_{u}, *σ*_{v}, *σ*_{w}, *σ*_{θ}, and *σ*_{q} calculated by the traditional EC
method for 30 min are all overestimated, especially when the turbulence is
weak, due to the impact of submesoscale motion. In addition, the
overestimation in the horizontal direction is more significant than in
the vertical direction. However, the overestimation of these quantities
cannot be ignored.

After separating pure turbulence and submesoscale motion from the signal, the pure turbulent flux can be calculated during heavy haze pollution periods. The comparison of the pure turbulent flux with the flux calculated by the eddy-correlation method at a fixed averaging time is presented in Fig. 5. The momentum flux, $-\stackrel{\mathrm{\u203e}}{{u}^{\prime}{w}^{\prime}}$, is overestimated by approximately 13 %, and the slope of the fitted line in Fig. 5c is approximately equal to 0.87. The effect of nonstationary motion on heat transfer and water-vapour transfer is similar to that on momentum, as seen in Fig. 5. Overestimation can reach 12 % (slope of 0.88) and 15 % (slope of 0.85) for $\stackrel{\mathrm{\u203e}}{{w}^{\prime}{\mathit{\theta}}^{\prime}}$ and $\stackrel{\mathrm{\u203e}}{{w}^{\prime}{q}^{\prime}}$ in Fig. 5a and b. The reconstructed turbulence data results at the urban site show that the traditional half-hourly eddy-correlation results have a certain degree of overestimation regarding the turbulent fluxes and variances during the pollution period. However, the degree of overestimation in urban areas is less than in suburban areas. A comparison of the macrostatistical parameters for turbulence from the new half-hourly results with those from the original results at the city site is not shown here.

In the majority of recent research, the EC technique has become the most
frequently used method with which to estimate the flux between land surfaces and the
atmosphere (Baldocchi, 2003). Under weak-stability conditions,
eddy-correlation fluxes calculated using a conventional averaging time of 5 min or longer to define the perturbations are severely contaminated by
poorly sampled mesoscale motions (Vickers and Mahrt, 2006). The average
block time that has been used is 30 min, which has been used in
practice since Kaimal and Finnigan (1994), who proposed that a 30 min
averaging time was a reasonable compromise for daytime analyses. From the
above analysis, we can see that turbulent fluxes are overestimated due to
the effects of submesoscale motions when there is a spectral gap. During the
heavy haze pollution process, turbulence is weak, which causes this
overestimation to become even more apparent. Zhong et al. (2017, 2018)
proposed that heavy pollution events in Beijing are characterized by the
transport stage (TS), with a formation of aerosol pollution primarily
caused by pollutants transported from regions south of Beijing, and the
cumulative stage (CS), where the cumulative explosive growth in PM_{2.5}
mass concentration is dominated by stable stratification characteristics in
the atmosphere, such as slight or calm southerlies, anomalous inversions
near the ground, and moisture accumulation. According to the classification
criteria for the CS and TS, we briefly compared the characteristics of
turbulent fluctuation, variance, and flux at different times during the
pollution process from 15 to 23 December 2016, as shown in Fig. 6.
Due to the consistent patterns of different variables, only the results for
horizontal velocity are shown in this paper. We can clearly see from Fig. 6
that the turbulent fluctuation, variance, heat flux, and momentum flux are
obviously smaller during polluted periods (CS and TS) than those during
clean periods. Therefore, the exchange of fluxes between the ground and
atmosphere can be easily overestimated with the traditional eddy-correlation
method during the pollution process, which can result in false forecasts of
contaminant concentrations and pollution levels. Some works have found that
current pollution forecasts tend to underestimate pollutant concentrations
(Li et al., 2016). The overestimation of turbulent flux during heavy
pollution episodes may be one of the reasons for this result.

After reconstruction via the automated algorithm, pure turbulent data can be obtained. The LIST from 16 December 2016 to 8 January 2017 is discussed in this section. We calculated the LIST of the urban and suburban sites separately and discussed the relationship between the LIST and degree of pollution.

Figure 7 shows the time series for (a) PM_{2.5} concentrations, (b) the
intermittency factor (IF) of vertical velocity, (c) the velocity scale for
submesoscale motions (*V*_{smeso}), (d) the velocity scale for turbulence
(*V*_{turb}), and (e) the LIST for turbulence from 16 December 2016 to
8 January 2017 at the suburban site. Figure 8 shows the results of the same
variables at the city site. Wei et al. (2018) has shown that there is a
relationship between the IF, which characterizes the intensity of
intermittent mixing, and the concentration of PM_{2.5}. In this section,
we also present the IF of the vertical wind speed in Figs. 7b and 8b to
discuss internal relations and differences with the local intermittent
strength. Low PM_{2.5} concentrations correspond to large values of IF,
*V*_{smeso}, and *V*_{turb}, and weak intermittent intensity (i.e., the LIST
is closer to 1) in Figs. 7 and 8. The decrease in PM_{2.5} concentration
corresponds to the increases in IF, *V*_{smeso}, and *V*_{turb} and
the decrease in local intermittent intensity. For several heavy pollution
events with PM_{2.5} concentrations higher than 200 µg m^{−3}, the
absolute value of the IF is smaller, the intensity of the submesoscale
motion is weaker than during the clean period, and the energy of the
turbulent flow is also weaker. Correspondingly, the local intermittent
intensity is strong, as the LIST is farther from 1. Specifically, for the
period of explosive growth in pollutant concentration (CS) during the two
pollution processes of Case I and Case II in Fig. 7, the intermittent
intensity (LIST) is significantly stronger (weaker) than during the
clean period and other weak pollution events, with a concentration of
approximately 200 µg m^{−3}. The two processes, Case I and Case II, are
similar in that both experience a rapid decline in the concentration of
PM_{2.5} (from a heavy pollution level greater than 500 µg m^{−3}
to one less than 30 µg m^{−3}) on a timescale of several hours. The
difference is that there is a clean period approximately 1 day after the
rapid decline in the Case I process, but in the Case II process, the
PM_{2.5} concentration decreases sharply in just a few hours and then
rapidly increases to the 600 µg m^{−3} level. By comparing the rapid
reduction in the PM_{2.5} concentrations during the Case I and Case II
processes, we find that there is no significant difference in submesoscale
motion strength, whereas turbulent intensity during the Case I process is
significantly greater than during the Case II process, which leads to a
weaker (stronger) LIST during the Case I (Case II). During the Case II
process, although the LIST (intermittent intensity) increases (decreases)
when the PM_{2.5} concentration begins to decrease, the larger (weaker)
LIST (intermittent intensity) is not maintained but decreases (increases)
rapidly, which indicates that the pollutant concentration does not fully
diffuse and rapidly increases again to 600 µg m^{−3} within a few
hours. The difference between these two processes also indicates that the
diffusion of pollutants directly depends on the diffusion of turbulent flow
during heavy pollution processes. Submesoscale motion may be an important
source of turbulent energy under stable weather conditions, but it is not
directly involved in the dissipation of pollutants.

From the analysis of the clean and polluted periods, we can see that the submesoscale motion persists throughout the 30 min acquired signal. During heavily polluted periods, the intensity of turbulence is weak, and the effects of submesoscale motion on weak turbulence begin to appear. During clean periods, the intensity of turbulence is strong, and the effect of submesoscale motion is relatively small. Meanwhile, the submesoscale motion is a source of turbulent energy when the turbulence is very weak under heavy pollution and stable weather conditions. It can be said that turbulence derives energy from nonstationary, large-scale motion and has a very large effect on the concentration of pollutants over timescales of hours (e.g., Case I and Case II). We also note the relationship between LIST and IF. Wei et al. (2018) mentioned that the larger the absolute value of the IF is, the stronger the intermittent mixing. From the perspective of intermittent mixing strength, the IF tends to be consistent with the LIST defined in this paper. When the pollutant concentrations decreased sharply, intermittent mixing increased, the IF absolute value increased, the LIST (intermittent intensity) increased (decreased), and turbulent exchange was enhanced.

The tendency of the LIST under pollution conditions in Fig. 8 is consistent
with that in Fig. 7, which indicates that the above analysis conclusions
apply not only to suburban sites but also to urban sites. However, there is
a significant difference between the urban and suburban sites: the LIST
(intermittent intensity) at suburban sites is weaker (stronger) than at
urban sites. The value of *V*_{smeso} at the city site is slightly smaller
than at the suburban site, and the value of *V*_{turb} at the city site
is larger than at the suburban site. Correspondingly, the value of the
LIST at the city site is significantly greater than at the suburban
site, which means that the dynamic effect of the underlying surface of the
urban area is stronger than that of the flat underlying surface of the
suburban area. Next, in Sect. 4.3 and 4.4, we verify the results from the
statistical characteristics of turbulence and the daily changes in turbulent
flux during polluted and clear periods, respectively.

Figures 9 and 10 show the relationship of the normalized standard deviations
in wind speed in the horizontal and vertical directions (${\mathit{\sigma}}_{u}/{u}_{\ast}$, ${\mathit{\sigma}}_{v}/{u}_{\ast}$, and ${\mathit{\sigma}}_{w}/{u}_{\ast}$) with potential
temperature (${\mathit{\sigma}}_{\mathit{\theta}}/\left|{\mathit{\theta}}_{\ast}\right|$) and moisture content (${\mathit{\sigma}}_{q}/\left|{q}_{\ast}\right|$) as functions of the
stability parameter *ζ* at the suburban site, respectively. It should
be noted that the reconstructions of the data have two benefits. One is that
the discrete situation of the fitted line has been significantly improved
after reconstruction. The other is that the statistical characteristics of
turbulence are more consistent with the classic statistical pattern for
turbulence, and the normalized standard deviations in potential temperature
and water vapour under near-neutral conditions are closer to those of
Panofsky et al. (1984) and Wyngaard (1971). The figures regarding the
macrostatistical characteristics of turbulence before reconstruction are not
shown here.

Figure 9 shows that under both polluted and clear weather conditions, the
relations of the normalized standard deviations in horizontal and vertical
wind speeds with the stability parameter *ζ* follows the one-third power law
well under stable and unstable stratification conditions. The normalized
standard deviation was more dispersed in the horizontal direction than
in the vertical direction, which is consistent with the results presented in
Zhang et al. (2004) and Ma et al. (2002) and shows that the physical
characteristics of the land surface (e.g., topography and roughness) affect
the statistical properties of the vertical wind speed less than those of the
horizontal wind speed. The normalized standard deviations in the horizontal
and vertical wind speeds are nearly constant under near-neutral conditions
(i.e., −0.01 < *ζ* < 0.01), and the constants are
slightly larger than those from Panofsky et al. (1984), which is similar to
the results from other suburban works (i.e., Zhang et al., 1991; Roth et
al., 1993; Su et al., 1994). Figure 9 shows that the values during
clean periods (circle) are slightly larger than those during haze periods
(asterisk) under unstable conditions. Ren et al. (2018) (Fig. 4) show the
significant difference in the normalized standard deviations in the
horizontal and vertical wind speeds between clear and haze periods. The
reconstructed data from the city site also show the same conclusion (the
figures are not shown in this paper), which means that the dynamic effect of
turbulence during pollution episodes is reduced significantly at both the
city and suburban sites. At the same time, the normalized standard
deviations in wind speed in three directions over the suburban area are
smaller than those over urban areas under near-neutral conditions, which
shows that the dynamic effect of turbulence at the urban site is stronger
than at the suburban site.

Figure 10 shows the relationships of the normalized standard deviations in
potential temperature and moisture with the stability parameter *ζ*.
Given unstable stratification, ${\mathit{\sigma}}_{\mathit{\theta}}/\left|{\mathit{\theta}}_{\ast}\right|$ and
${\mathit{\sigma}}_{q}/\left|{q}_{\ast}\right|$ fit the
function ${\mathit{\zeta}}^{-\mathrm{1}/\mathrm{3}}$. The fitting coefficients are larger than the
typical value of 0.95 presented in Wyngaard (1971), which used data from a
grassland area in Kansas (United States). Similarly to the conclusion for the
normalized standard deviations in the three-directional wind speeds, Ren et
al. (2018) (Fig. 5) shows the slight differences in the normalized standard
deviations in potential temperature between clear and haze periods, while
Fig. 10 in this paper shows a significant difference between clear and haze
periods. Since the time periods studied are the same, the difference in the
performance of these turbulence statistics during polluted and clean periods
over city and suburban sites indicates the impact of urbanization. In other
words, the pollution process has a more significant influence on the
turbulent statistical characteristics of potential temperature and moisture
in the suburbs and a less significant impact on those in the urban area.

Figure 11 shows the diurnal variations in the mean $\stackrel{\mathrm{\u203e}}{{w}^{\prime}{\mathit{\theta}}^{\prime}}$,
$\stackrel{\mathrm{\u203e}}{{w}^{\prime}{q}^{\prime}}$, $-\stackrel{\mathrm{\u203e}}{{u}^{\prime}{w}^{\prime}}$ and TKE under both polluted
weather and clear weather conditions. The sensible heat flux (vertical heat
flux) exhibits unimodal diurnal variations during both clean and polluted
periods over either the suburban site or city site, as shown in Fig. 11a
and e. During the clean period, the peak in the daily sensible
heat flux at the suburban site appears around 12:00 noon (local time), reaching
a maximum of 0.07 K m s^{−1}; the peak in the daily sensible heat flux at
the urban site also appears around 12:00 noon, with a peak value close to 0.04 K m s^{−1}, which is less than that in the suburban area. One possible
reason is that the buildings in the urban area are denser and have higher
reflectivity, resulting in less net radiation and, consequently, a lower
peak in the sensible heat flux. Another difference in the sensible heat flux
between the city and suburban sites during the clean period is that the
sensible heat flux over the suburbs is negative at night, with a downward
heat transfer, but not in urban areas. This pattern may be due to the
emission of anthropogenic heat sources at nighttime in cities and the
difficulty of dissipating heat over tall and dense buildings; therefore,
there is not a vast temperature difference between the surface of the city
and the upper air and, accordingly, the sensible heat flux is not completely
below zero. Previous research on city and suburban sites in Helsinki
also found the same features (Nordbo et al., 2013). During the pollution
period, the peak in sensible heat flux at the urban site dropped to
approximately 0.02 K m s^{−1}. In addition, other trends were exactly the
same as those during the clean period. At the same time, the peak in
sensible heat flux at the suburban site dropped to 0.02 K m s^{−1}, and
the daily change in sensible heat flux was somewhat different than
during the clean period (i.e., the characteristic of downward sensible heat
flux at night disappeared completely). In general, pollution caused a
reduction in the upward transport of sensible heat flux, and it had a weaker
impact on the city and a stronger impact on the suburbs. In addition,
pollution can also hinder the downward transmission of nighttime sensible
heat flux in the suburbs.

The daily changes in latent heat flux over the urban and suburban areas are completely different. During the clean period, the latent heat flux at the city site (Fig. 11b, dotted line) does not have obvious daily variations and fluctuates at approximately 0, which is related to low winter temperatures, the presence of water in the form of solid ice, and very dry air. However, the daily changes in latent heat in the suburbs during the clean period show a unimodal change, reaching a peak at approximately 12:00 noon. It seems that the pollution process has no significant effect on the transport of latent heat over the urban area. As the solid line in Fig. 11b shows, the latent heat flux over the urban area during the pollution period remains low, fluctuating at approximately 0. However, the pollution process has a greater impact on the transfer of latent heat in the suburbs. As shown by the dotted line in Fig. 11f, the transfer of latent heat is reduced throughout the day.

The magnitude of the momentum flux is related to the roughness of the underlying surface, wind speed, and stability of the boundary layer. During the clean period, the momentum flux over the city site experiences a wide range of changes, and the peak value is larger due to the high roughness of the city's underlying surface; the suburban momentum flux also has obvious daily changes, but the peak value is slightly lower than over the city site. During the pollution period, the momentum fluxes at the urban and suburban sites are significantly lower than those during the clean period and remain low throughout the day. However, at this time, the momentum flux over the city is greater than over the suburbs, as Fig. 11c and g show. The change in TKE is similar to that in momentum flux. During the clean period, the TKE values over the urban and suburban sites all showed obvious unimodal diurnal variations. The TKE values over the urban area were greater than those over the suburban area, which is due to the strong turbulence in wake vortices caused by underlying surfaces, such as high buildings in urban areas. During the pollution process, the urban and suburban TKEs both decreased significantly and remained low throughout the day. However, the TKE over the city site was still greater than over the suburban site.

Based on the above analysis, we know that the sensible heat flux and latent heat flux of the urban site are less than those of the suburban site, and the momentum transport and TKE of the urban areas are greater than those of the suburban sites due to different underlying surfaces. The sensible heat flux, latent heat flux, momentum flux, and TKE in the urban and suburban areas are all affected when pollution occurs. Pollution inhibits the material and energy exchanges between the surface and atmosphere. Moreover, the impact of the pollution process on the suburbs is much greater than on the urban area. If the turbulent structure over the flat surface of the suburban area is considered the normal state for turbulent structures in this area during the studied period, then the urban turbulent structure is influenced by urbanization. From this perspective, urbanization has reduced the impact of pollution on water and heat exchanges between the surface and atmosphere. In conjunction with Sect. 4.2, the value of the LIST in urban areas is greater than in suburban areas, which means that the intermittent intensity of urban turbulence is less than that of suburban turbulence. Therefore, the turbulence signal over the urban site is stronger than over the suburban site, and pollution in urban areas is weaker than in adjacent suburbs.

5 Conclusions and discussions

Back to toptop
In this paper, we developed an automated algorithm to identify the spectral
gap to separate pure turbulence and submesoscale motions from a 30 min
signal based on the arbitrary-order Hilbert spectral method. We used this
automated algorithm to analyse turbulence data observed from several severe
haze pollution episodes in Beijing and its nearby suburbs from 16 December 2016 to 8 January 2017. The data sets with a spectral gap accounted for
approximately 30 % of the total data, indicating that the eddy-correlation
flux calculated using a conventional averaging time of 30 min to define
perturbations is severely contaminated by poorly sampled mesoscale motions.
Due to space limitations, only the detailed suburban site results are listed
in the text. The results of the urban site are consistent with the
conclusions of the suburban site. A comparison between the reconstructed
variances of *u*^{′}, *v*^{′},
*w*^{′}, *θ*^{′}, and
*q*^{′} and those calculated by the conventional method
revealed overestimations of approximately 27 %, 21 %, 1 %, 40 %, and
46 %, when there was a spectral gap. The vertical wind speed
was overestimated less than the horizontal wind speed. The scalar, potential
temperatures were overestimated more than the wind speed vector. The
calculations of the fluxes were also overestimated. The momentum flux, heat
flux, and water-vapour flux were overestimated by approximately 13 %,
12 %, and 15 %. We can see from these comparisons that the
overestimation of flux during haze events cannot be ignored.

After reconstruction via the automated algorithm, pure turbulent data can be obtained. Then, we explore the relationship between the LIST and pollution. The results indicate that, when pollution is heavy, the LIST is smaller, and the intermittency is stronger; when pollution is lighter, the LIST is larger, and the intermittency is weaker. During the heavy pollution process, air quality is determined by turbulent motion on the hourly scale. At the same time, the LIST at the city site is greater than at the suburban site, which means that the intermittency over the complex city surface is weaker than over the flat terrain of the suburbs. Urbanization seems to reduce the intermittency during heavy haze pollution episodes. The results were validated via the statistics on the impact of urbanization on turbulence and turbulent transport during polluted and clean periods.

The results for the statistical characteristics of turbulence show a significant difference in the normalized standard deviations in the horizontal and vertical wind speeds between clear and haze periods at the suburban site, which is the same as that at the city site; significant differences in the normalized standard deviations in potential temperature and water-vapour content between clear and haze periods are also observed at the suburban site, which are substantially different from those at the city site. These conclusions are consistent with the diurnal variations in mean flux under both polluted weather and clear weather conditions at the city site and suburban site. The sensible heat flux, latent heat flux, momentum flux, and TKE over the urban and suburban areas are all affected when pollution occurs. Due to the close distance between the two stations, the large-scale weather background is consistent, and the suburban site is locally flat, so the turbulent structure over the flat surface of the suburban area is considered the normal state in this area under such weather and pollution source conditions; then the urban turbulent structure is influenced by urbanization. More importantly, the reduction in turbulence exchange during the pollution period in suburban sites is greater compared to urban sites. In other words, the impact of the pollution process on the suburbs is much greater than on the urban area. The change in the underlying surface of the urban site (the dynamic effect of complex terrain and the heat island effect caused by human activities) leads to a greater resistance to the weakening effects of turbulent exchange caused by pollution.

Data availability

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Data availability.

Data used in this study are available from the corresponding author upon request (hsdq@pku.edu.cn).

Author contributions

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Author contributions.

YR and HZ determined the goal of this study. YR carried it out, analyzed the data and prepared the paper with contributions from all co-authors. WW helped to figure out the methodological problem based on HHT. BW, XC and YS designed the field experiment, carried them out and got the data. All authors contributed to the discussion and interpretation of the results and to article modifications.

Competing interests

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Competing interests.

The authors declare that they have no conflict of interest.

Acknowledgements

Back to toptop
Acknowledgements.

This work was jointly funded by grants from National Key R&D
Program of China (2016YFC0203300) and the National Natural Science Foundation
of China (91544216, 41705003, 41675018, 41475007).

Edited by: Jianping Huang

Reviewed by: two anonymous referees

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Short summary

During the heavy pollution process, there are overestimations regarding the exchange between the atmosphere and surface since the normal calculation of turbulent fluxes includes the impact of sub-mesoscale motion. The intermittent turbulence intensity is closely related to the concentration of PM2.5. The intermittency is weaker over the complex surface condition than over the flat terrain, and urbanization reduces the degree of weakening in turbulent exchange during the heavy pollution process.

During the heavy pollution process, there are overestimations regarding the exchange between the...

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