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Atmospheric Research 231 (2020) 104675

Contents lists available at ScienceDirect

Atmospheric Research
journal homepage: www.elsevier.com/locate/atmosres

On the association between characteristics of the atmospheric boundary T


layer and air pollution concentrations

Yuvala, , Yoav Levib, Uri Dayanc, Ilan Levyd, David M. Brodaya
a
Department of Civil and Environmental Engineering, Technion, Israel Institute of Technology, Haifa 32000, Israel
b
Israel Meteorological Service, P.O. Box 25, Bet Dagan 5025001, Israel
c
Department of Geography, The Hebrew University of Jerusalem, Jerusalem 9190501, Israel
d
Air quality and climate change division, Ministry of Environmental Protection, 125 Menachem Begin road, Tel Aviv 61071, Israel

A R T I C LE I N FO A B S T R A C T

Keywords: Air pollution in the lower atmosphere is a global concern. Characteristics of the planetary boundary layer (PBL)
Air pollution are considered important determinants of the dispersion and the concentrations of pollutants. This work explores
Convective boundary layer the association between characteristics of the PBL and corresponding air pollution data, separately for different
Residual boundary layer PBL states. Five years (2014–2018) of twice daily (01:30 and 13:30 local time) high resolution radiosonde data
Stable boundary layer
were used to estimate the convective and stable boundary layer heights (CBL and SBL, respectively), and the
Temperature lapse rate
temperature lapse rate, in Bet Dagan, Israel. In 23% of the nights, mostly cloudy ones, no indication for an SBL
was found but a clear top of a ground–based residual layer (RBL) was detected. The concentrations of NO, NO2,
NOx and PM2.5 were negatively correlated with the heights of the CBL and RBL but positively correlated with the
SBL height. Their association with the lapse rate was always negative, weak in daytime (CBL) but very strong
during the night (SBL and RBL). The associations with the O3 concentrations were opposite in sign to those with
the primary pollutants. The PBL height using the bulk Richardson number method was most strongly associated
with the CBL and RBL concentrations but we found it unsuitable for estimating the height of the SBL. Our results
demonstrate the importance of accounting for the different states of the PBL. In particular, they suggest that
during SBL conditions, the common practice of using the PBL volume as a determinant of pollutant con-
centrations might not be appropriate.

1. Introduction Tennekes, 1984; Vogelezang and Holtslag, 1996), with verification of


the theoretical formulations usually based on the few available sources
The planetary boundary layer (PBL) is the lowest part of the at- e.g., the Wangara field experiment in Australia (Yu, 1978) and the
mosphere through which the Earth's surface exchanges mass, mo- Cabauw tower measurements in the Netherlands (Vogelezang and
mentum and heat with the free atmosphere. In clear weather conditions Holtslag, 1996). In other cases, the PBL parameters were extracted from
daytime surface heating generates convection and the build up of a model output (e.g., Lieman and Alpert, 1993). The 21st century has
convective boundary layer (CBL). Radiation cooling during the night seen an explosive increase in modern measurement methods for
results in stable atmospheric conditions, and the creation of a stable studying the PBL, and in the amount of available data. Radiosonde
boundary layer (SBL) close to the surface below a residual of the pre- profiling is still the main operational tool (e.g., Seidel et al., 2010;
vious day CBL aloft (Fernando and Weil, 2010; Klein et al., 2016). In the Seidel et al., 2012; Guo et al., 2016; Miao et al., 2018), carried out
middle and lower latitudes, the morning transition between SBL to CBL global–wide in thousands of locations, usually twice daily. They are
conditions is quick and occurs shortly after sunrise (Taylor et al., 2014). corroborated by field campaigns of in–situ measurements using teth-
The late evening transition from CBL to SBL can be slow, especially in ered balloons and aircraft (Dayan et al., 1988; Balsley et al., 2006;
urban setting where the urban heat island counteracts the radiation Balsley et al., 2008; Pournazeri et al., 2012). The emergence of remote
cooling (Sarrat et al., 2006; Taylor et al., 2014). sensing instruments based on acoustic properties (SODAR, Emeis and
Many studies examined various aspects of the PBL. Early works Schäfer, 2006, Neves and Fisch, 2015), optical properties (Ceilometer,
were mainly theoretical (e.g., Tennekes, 1973; Yu, 1978; Driedonks and Emeis and Schäfer, 2006; Wagner and Schäfer, 2017), aerosols


Corresponding author at: Department of Civil and Environmental Engineering, Technion, I.I.T., Haifa 32000, Israel.
E-mail address: lavuy@tx.technion.ac.il (Yuval).

https://doi.org/10.1016/j.atmosres.2019.104675
Received 8 April 2019; Received in revised form 4 September 2019; Accepted 6 September 2019
Available online 09 September 2019
0169-8095/ © 2019 Elsevier B.V. All rights reserved.
Yuval, et al. Atmospheric Research 231 (2020) 104675

concentration gradients (LIDAR, Hennemuth and Lammert, 2006; 2.2. Data


Kotthaus et al., 2018; Xiang et al., 2019) and the Doppler effect (wind
profilers; Uzan and Alpert, 2012) enables continuous measurements of 2.2.1. Radiosonde and meteorological data
the PBL height but usually in a limited number of locations and/or for a A radiosonde is a telemetry instrument which is lifted up from the
limited period of time. ground by a weather balloon and transmits to a base station continuous
Most of the PBL studies mention its association with air pollution as measurements of the atmosphere. We used data of a radiosonde laun-
a major motivation. For example, the often cited review by Siebert et al. ched twice daily around 01:30 and 13:30 local standard time
(2000) on the determination of the PBL height was initiated as a result (UTC + 2 h), by the Israeli Meteorological Service (IMS) following in-
of the need to improve air quality assessments. PBL characteristics, ternational standards. The launching site is in the IMS premises (long-
mainly its height, are used as an important input to air quality models. itude 34.81E, latitude 32.0 N) at elevation of 31 m above sea level. It is
Kotthaus et al. (2018) emphasise that the PBL volume is critical for about 7 km southeast of the centre of the Tel Aviv metropolitan area,
assessment of air quality. Surprisingly, the number of studies that ac- 7 km east of the shoreline and 3.5 km west of the western edge of the
tually examined the association of PBL characteristics and air pollution Ben Gurion international airport perimeter (Fig. 1). Due to the airport
concentrations is limited. Several studies investigated the PBL height proximity and associated safety issues, actual launch time may vary by
during severe air pollution events (Liu and Chan, 2002; Dupont et al., up to an hour from the scheduled one. The observations are logged
2016; Xiang et al., 2019). Uzan and Alpert (2012) and Nair et al. (2018) every two seconds, which with average balloon vertical speed of 5 ms−1
studied the long term impact of daytime PBL height on the concentra- results in about 10 m vertical resolution. Quite significant variations in
tions of several pollutants at shoreline locations, while Wagner and the ascent rate may occur in the first few second immediately after the
Schäfer (2017) studied the PBL impact in a street canyon scenario. radiosonde launch. The variables observed by the radiosonde are height
Recent papers by Miao et al. (2018) and Liu et al. (2018) examined the above ground level, barometric pressure, temperature, relative hu-
relationship between the PBL height and PM2.5 concentrations in cities midity, wind speed and wind direction. The Väisälä Radiosonde RS92-
in China. The association of the temperature lapse rate, a measure of SGP was used until November 2016 and the RS41-SG model has been
atmospheric stability in the PBL, and air pollution concentrations was used since then. The instrumentation is calibrated before each launch.
studied by Han et al. (2009) and Grundström et al. (2015). Most of the The temperature response time (63.2%, 6 ms−1 flow and 1000 hPa) is
studies which examined associations between PBL characteristics and less than 0.5 s and reproducibility is 0.15 °C.
air pollution considered either the CBL (Uzan and Alpert, 2012; Nair Surface meteorological data were obtained from the permanent
et al., 2018), the SBL (Han et al., 2009) or used methods that do not meteorological station located at the IMS premises. The station observes
specify the state of the PBL (Wagner and Schäfer, 2017; Miao et al., at a 10-min temporal resolution the temperature, relative humidity,
2018; Liu et al., 2018). solar radiation and precipitation at a height of 2 m a.g.l., and the 20 m
This work explores the association between two PBL character- a.g.l. wind direction and speed. Cloud cover is observed in the same
istics–its height and lapse rate–and the concentrations of several air location on an hourly basis and we used the observations at 00:00 and
pollutants, making the distinction between different states of the PBL. 12:00, local time. The IMS assigns the permanent meteorological sta-
Several methods for PBL height determination were employed and their tion data to the first (zero seconds) radiosonde record at the time of
association with air pollutant concentrations were compared. Our re- launching. Due to some large inconsistencies, the first radiosonde re-
sults contribute to understanding of the role of the PBL in determining cord was ignored and the second (two second from launching, on
ambient pollutant concentrations. Practical implications for pollution average at a height of 6.2 m) was always considered as the reference.
level assessments are discussed.
2.2.2. Air pollution data
The air pollution data used for this study were obtained from the
2. Materials and methods Israeli air quality monitoring array, operated under the supervision of
the Israeli Ministry of Environmental Protection. The stations use
2.1. Study area standard and USEPA approved instrumentation and their operation
procedures follow EPA guidelines. The records are available at a
The study area is in central Israel, a few km from the Mediterranean half–hourly temporal resolution and the data at the half–hourly time
shoreline (Fig. 1). It is characterised by long, dry, hot and mildly humid point closest to the actual radiosonde launch were assigned to it for
summers (daily mean temperature and relative humidity 25 °C and joint analyses. Automatic calibration is carried out in the stations on a
65%, respectively), with intense solar radiation during the day (up to daily basis in the early hours after mid–night and data are not logged
1250 Wm−2) and rapid cooling during the mostly clear nights. Winters during this time. The selected air quality monitoring stations were those
are mild (mean daily temperature 14 °C), with the weather dominated closest to the radiosonde site and which had their calibration done in
by irregular succession of high pressure systems, Red Sea troughs (a hours not coinciding with the time window of the radiosonde
northward extension of the Sudan monsoon low), both usually result in launching. NO, NO2, NOx and PM2.5 data are from the Holon station,
clear weather, warm days and cold nights, and eastern Mediterranean situated at the top of a school building, 16 m above ground, 1.1 km east
cyclonic systems, which result in cold weather and most of the annual of Tel Aviv's main transportation artery and 5 km west of the radio-
precipitation (long term annual mean of 520 mm). sonde launching site (Fig. 1). The main local source of PM and nitrogen
Locally generated NOx and particulate matter (PM) are mainly due oxides is traffic. Data from Decell LTD., which is based on continuous
to transportation, with additional NOx contributions from a natural onboard vehicle GPS readings (Chen et al., 2016), indicate that traffic
gas–fired power station (peak capacity of 428 MW) at the shoreline and volume in the 250 × 250 m area around the monitoring station
a cement production plant east of the study location. The background amounts during working days to about 1000 cars and 50 trucks per
ozone levels are titrated by locally produced NOx and VOCs, resulting in hour at the mean hour of daytime radiosonde launch, and to about 400
relatively low ozone level in the study area and high ozone level cars per hour and close to zero trucks at the mean hour of the night-time
downwind. Particulate matter has additional external sources. The launch. The weekend private car volumes are about half of the week-
major one is transport of secondary PM from Europe (Dayan and Levy, days averages, with very little or zero weekend truck traffic. The O3
2002; Asaf et al., 2008). In addition, naturally occurring mineral dust data are observed at the Ahisemech station, located on the ground in an
arrives at the area, usually between October to May, by long range agricultural community at the southeastern edge of the Tel Aviv me-
transport from the surrounding deserts (Yuval et al., 2015), and is also tropolitan area, about 18 km from its centre and 12.7 km southeast of
generated locally by wind associated with winter storms. the radiosonde launching site (Fig. 1).

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Yuval, et al. Atmospheric Research 231 (2020) 104675

Fig. 1. Left panel: location of the study area in central Israel. Right panel: Locations of the measurement sites. The Bet Dagan radiosonde launching site is marked by a
triangle. The circle marks the location of the Holon air quality station where the NO, NO2, NOx and PM2.5 concentrations were observed and the square marks the
location of the Ahisemech air quality station which observed the O3 concentrations. Dark shadings denote residential areas, the light shading east of the Bet Dagan
launching site marks the airport and the red lines are major highways. The coordinates are of the Israeli New Grid projection in metres. (For interpretation of the
references to colour in this figure legend, the reader is referred to the web version of this article.)

2.3. Analysis methods which is based on integrating the temperature and humidity informa-
tion using four widely used CBL height estimation methods (e.g., Seidel
2.3.1. Initial processing et al., 2010).
All the data sets went through a quality assurance process to detect The Richardson number is the ratio of turbulence associated with
and eliminate erroneous data. Many radiosonde records during a buoyancy to that associated with mechanical shear. In unstable condi-
transition period in the logging software and instrumentation towards tions it is expected to be negative or small. Close to the CBL top it is
the end of 2016 were found to be corrupt. Thus the data from 17 expected to exceed the critical value of 0.25, above which the atmo-
November 2016 to 31 December 2016 were not used. A small percen- spheric flow is considered laminar. The bulk Richardson number Rib
tage (< 1%) of the air pollution and meteorological data with values (Eqs. 8 and 9 in the Supplementary Material) is a bulk measure of an
beyond their physical range or showing variability not fitting the atmospheric layer. Following Seidel et al. (2012), Guo et al. (2016),
measured variable were designated as missing. The observed radio- Miao et al. (2018) and Liu et al. (2018), we calculated Rib by con-
sonde data were used to calculate a few additional variables needed for sidering successively for each radiosonde elevation level the layer be-
the PBL height determination: the potential temperature Θ, virtual tween it and the surface. The CBL height hcblRb was determined as the
potential temperature Θv, water vapour mixing ratio w, the gradient elevation where Rib ≥ 0.25 for the first time. We tested also a similar
Richardson number Rig and the bulk Richardson number Rib. The procedure using the gradient Richardson number (see eq. 7 in the
mathematical formulae used to calculate these variables are provided in Supplementary Material) but it's vertical profile was too erratic to re-
the Supplementary Material. liably estimate the CBL height.
The W&W procedure considers as initial candidates for the CBL
height the elevations of the maximum vertical gradient of the potential
2.3.2. Determination of the temperature lapse rate and the PBL height
temperature, and of the minima of the vertical gradients of the relative
The temperature lapse rate is the change in the observed tempera-
humidity, specific humidity and the atmospheric refractivity (Smith
ture while moving upward through the Earth's atmosphere. It de-
and Weintraub, 1953; Seidel et al., 2010; Wang and Wang, 2014).
termines the atmospheric stability and thus the vertical dispersion of
According to the W&W method the CBL height hcblW is defined as the
pollutants emitted at the surface. The temperature lapse rate was de-
mean value of at least three of these candidate values which are within
fined as Γ = − ΔT/Δz where ΔT and Δz are the differences in tem-
less than 50 m one from the others. We adopted the Wang and Wang
perature and radiosonde elevation, respectively, between a certain
(2014) procedure with some modifications specified in the Supple-
elevation after launching the radiosonde and the second radiosonde
mentary Material.
reporting level (two second from the launch, on average at z = 6.2 m).
Two different methods were used to estimate the SBL height: (a) the
The lapse rate was always assigned to the radiosonde elevation z, and
temperature method, which considers the height of the surface tem-
we studied the lapse rate considering a range of fixed elevation levels.
perature inversion, i.e. the elevation where the positive temperature
In daytime we also considered the laspe rate between the surface and
gradient (temperature increasing with height) near the ground becomes
the top of the superadiabatic part of the CBL.
negative (Yu, 1978; Seidel et al., 2010; Pournazeri et al., 2012); and (b)
The CBL height was estimated using two different procedures: the
the Richardson number method. Given the high resolution of our
bulk Richardson number method (Vogelezang and Holtslag, 1996;
radiosonde data we considered the gradient Richardson number (hen-
Seidel et al., 2012; Guo et al., 2016; Liu et al., 2018; Miao et al., 2018)
ceforth Rig; Ohya, 2001, Zilitinkevich and Baklanov, 2002; Galperin
and the Wang and Wang (2014, henceforth called the W&W) method,

3
Yuval, et al. Atmospheric Research 231 (2020) 104675

et al., 2007) whereas previous studies which examined the association Richardson number increases with height. Upside–down SBL was as-
between the PBL and air pollution used the bulk Richardson number sociated with very stable conditions (Ohya, 2001) and indeed, the Rig
(Seidel et al., 2012; Guo et al., 2016; Liu et al., 2018; Miao et al., 2018), profile in Fig. 3b resembles in shape the profiles of Rig associated with
designed to be used with data at coarse vertical resolutions. We noticed high stability shown in Fig. 6 of Ohya (2001). Fig. 3c shows the cor-
mostly very stable conditions within the SBL, with high values of Rig responding Rib profile, with values smaller than the critical value at the
close to the surface, decreasing with height to the critical value of 0.25. surface but exceeding it at an extremely low elevation (13 m in this
This usually implies an upside down SBL (Mahrt, 1999; Ohya, 2001; case). The shapes of the Rig and Rib profiles shown in Fig. 3 are very
Mahrt and Vickers, 2002) and we considered its top to be the level at typical and appear in most cases when an SBL was detected.
which Rig ≤ 0.25. We also implemented the bulk Richardson method to Fig. 4 shows a typical example of a night-time launch when an SBL
determine the SBL height but, as will be shown below, it proved un- was not present but a top of a ground–based RBL was detected. The
suitable for this purpose given the stability conditions in our study area. gradient of the temperature in Fig. 4a is negative and small in absolute
The existence of a surface temperature inversion is a clear indication terms compared to the strong positive surface gradient of the tem-
of a stable atmosphere. In all cases (both day and night) when it was perature profile shown in Fig. 3a, where SBL conditions were detected.
detected, the PBL state was designated as SBL with height estimated by In Fig. 3b the Rig profile reaches very high values (stable conditions)
hsblT (temperature method) and hsblRg (gradient Richardson number before decreasing below the 0.25 critical value at an elevation close to
method). When an SBL was not detected in a daytime record (the great that of the surface temperature inversion. In Fig. 4b on the other hand,
majority of cases) but a CBL was, the PBL state was designated as CBL, small values of Rig fluctuate wildly around the critical value. Fig. S3
with height estimated by hcblW and hcblRb. In cases of night-time launch shows the RBL height detected in the data of this launch using the Rib
not indicating existence of SBL but with a clear PBL top detected using and W&W methods. Typical to RBL conditions, the RBL top determined
the W&W method, we considered the situation to be a residual by the Rib method in this case is much lower than the one determined
boundary layer under which an SBL has not yet developed, henceforth by the W&W procedure (193 m vs. 826 m, respectively).
designated as an RBL, with estimated height hrblW or hrblRb. Table 2 provides descriptive statistics of the PBL characteristics. The
All the initial processing of the data, determination of the PBL lapse rate statistics in the table use the data of the 12th radiosonde
characteristics, and the subsequent analyses were carried out by auto- reporting level (24 s from launch, on average at 108 m). Lapse rates
matic procedures coded using Matlab (Matlab, 2018) version calculated for lower (higher) elevations are more (less) extreme. The
9.4.0.813654. statistics of the 108 m lapse rate are presented due to the proximity of
this elevation to the typical heights of both the SBL and the CBL's su-
peradiabatic sub–layer. We found that the 108 m lapse rate is always
3. Results strongly positive during daytime CBL conditions, being superadiabatic
in 90% of the cases. During RBL conditions, both positive and negative
Table 1 provides information about the number of successful laun- lapse rates occur, with a median of 3.4 °C km−1. When an SBL devel-
ches, valid records and the number of different PBL state occurrences oped at night, in 98% of the cases the surface to 108 m lapse rate was
during the study period. The number of daytime and night-time laun- negative, with very wide distribution reaching rates of −110 °C km−1.
ches in the 1826 days of the study period were, respectively, 1812 and In the remaining 2% cases the SBL height was much lower than 108 m,
1814, out of which 1768 and 1773 launches were found to have valid with the lapse rate below it negative. As expected, the CBL height is
records. During daytime, CBL was detected in 81.3% of the launches significantly higher than the height of the SBL. The highest PBL levels
and 18.7% of the time PBL was not detected (e.g., due to lack of were estimated by the W&W method during RBL conditions. Interest-
agreement among at least three of the methods used by the W&W ingly, while the CBL heights by the W&W and the Rib methods are
procedure). We ignored and have not used in any of the analyses the comparable, during RBL conditions the Rib method results in much
five cases of daytime SBL detections. During night-time, SBL and RBL smaller values. The SBL height using the temperature method is larger
were detected in 70.8% and 24.2% of the launches, respectively, and than the height obtained by the Rig method in about 50% of the time.
5% of the time PBL could not be detected. However, the SBL height using the temperature method has a dis-
Figs. 2 and 3 show, respectively, typical examples of vertical profiles tribution with a very long right tail which results in 20%–30% higher
of the meteorological variables used for the CBL and SBL height de- mean and corresponding percentiles. Both methods found a significant
termination. Some of the PBL height determination methods use the number of SBL heights below 50 m (12% and 19% of the cases for the
gradients of the variables and Figs. S1 and S2 in the Supplementary temperature and Rig methods, respectively). Such low PBL height could
Material show the same examples but with the gradients of the vari- not be resolved by the coarse resolution radiosonde data very often
ables also plotted. In Fig. 2 the CBL heights determined by all the five used for PBL climatological studies (e.g., Seidel et al., 2012). In more
methods are very similar (804, 763, 790, 790 and 790 m for the Rib, Θ, than 10% of the cases the Rb value at the surface was already larger
RH, w and N methods, respectively), with the height by the Rib method than the critical value, effectively indicating zero SBL height. Moreover,
slightly higher than that by the W&W procedure. In Fig. 3 it is im- in 30% of the cases the SBL height using the Rib method was less than
portant to note the high values of the gradient Richardson number (i.e., 10 m. This suggests that the Rib method is not appropriate for de-
stable conditions) before its first decrease below the critical value of termination of the SBL height in our study area and thus in the fol-
0.25. This might imply an upside–down SBL, where the turbulence lowing the Rib method is considered only for CBL and RBL conditions.
transport is downwards towards the surface (Mahrt, 1999; Ohya, 2001; Table 3 provides the median values of meteorological variables
Mahrt and Vickers, 2002; Klein et al., 2016), opposite to the case of observed during the radiosonde launch times for each of the three PBL
traditional SBL where the turbulence is generated at the surface and the states. CBL conditions, exclusively at daytime, are characterised by low
cloud cover, high temperatures and fast warming, medium relative
Table 1 humidity, high wind speed and a high standard deviation of the wind
The number of successful launches, valid records and the PBL state occurrences
direction, the latter pointing to considerable turbulence. The night-time
in the 2014–2018 study period. According to our definitions, CBL can occur
SBL conditions are characterised by mostly clear skies, cold tempera-
only in daytime and RBL only at night.
tures with fast cooling rate, high relative humidity, low wind speed and
Launches Valid records PBL detected CBL RBL SBL low standard deviation of the wind direction. The RBL is also a night-
time phenomenon but it occurs more often in summer time (Fig. S4 in
Day 1812 1768 1443 1438 NA 5
Night 1814 1773 1685 NA 429 1256 the Supplementary Material), which explains the much higher tem-
peratures compared to SBL conditions. However, it is important to note

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Yuval, et al. Atmospheric Research 231 (2020) 104675

a b c d e
1000 1000 1000 1000 1000

800 800 800 800 800

600 600 600 600 600


Z(m)

400 400 400 400 400

200 200 200 200 200

-4 -2 0 2 28 30 32 40 60 6 8 10 12 280 300 320 340


Rib ( oC ) RH (%) w (g/kg) N

Fig. 2. Vertical profiles of the bulk Richardson number Rib, potential temperature Θ, relative humidity RH, mixing ratio w and the refractivity N on 1 July 2014 at
12:32 (local time). The CBL height detected using each of the profiles is marked by a thin dashed horizontal line. The thick dashed line is the CBL height hcblW,
determined as the mean of the heights detected by the Θ, RH, w and N methods (W&W method). The dotted vertical line in panel (a) denotes the 0.25 critical
Richardson number, which determines the CBL height using the Rib method.

that the RBL is also characterised by significantly higher cloud cover, (see Fig. S4 in the Supplementary Material). The annual cycle of the
much slower cooling rate, higher wind speed and much higher standard RBL height seems to follow that of the CBL but with heights a few
deviation of the wind direction, all discouraging generation of stable hundred metres larger. The annual cycle of the lapse rate during RBL
atmospheric conditions. has no clear pattern and is characterised by magnitudes much smaller
The monthly medians of the PBL height (W&W method for CBL and compared to the CBL and SBL lapse rates.
RBL conditions, temperature method for SBL conditions), and the cor- Fig. 6 shows the monthly medians of the air pollutants during CBL,
responding lapse rate between the 12th radiosonde reporting level RBL and SBL conditions. Only data from working days (Sunday to
(average of 108 m) and the surface are shown in Fig. 5. The CBL and Thursday in Israel) were used to avoid confounding due to the reduced
SBL heights, and their corresponding lapse rate values show clear an- local emissions in weekends and holidays. Very significant differences
nual cycles (Fig. 5a and Fig. 5c, respectively). In both cases the corre- can be noted between the curves of each pollutant for different PBL
lation between the PBL height and the lapse rate is negative, with lar- states in terms of both concentration levels and annual cycles. While
gest CBL and SBL heights during winter while the corresponding lapse PM2.5 concentrations during the day (i.e., CBL conditions) vary incon-
rates are smallest. The lowest mean CBL heights are found in spring sistently between 15 and 20 μgm−3, the night-time concentrations re-
time (April), probably due to a large sea to land temperature gradient veal clear annual cycles, with highest (lowest) concentrations during
and the resulting intense sea breeze, promoting lower CBL. The SBL (RBL) conditions in the winter. The 15 μgm−3 difference in the
minimum of the monthly median SBL height is in July, and the lapse January PM2.5 concentration between these two night-time PBL states is
rate maximum values are in July and August. The monthly median on the order of the total PM2.5 annual mean, demonstrating the po-
curves of the RBL height and its corresponding lapse rate are jittery tentially high impact of the prevailing PBL state in determining the
(Fig. 5b), probably due to the small monthly sample sizes of the RBL night-time PM2.5 concentration. On the other hand, PM2.5 concentration

Fig. 3. Vertical profiles of the temperature, gradient Richardson


a b c number Rig and the bulk Richardson number Rib on 1 January 2014 at
300 300 300 01:43 (local time). The SBL height detected using each of the profiles
is marked by a dashed horizontal line. The dotted vertical lines denote
the 0.25 critical Richardson number, which determines the SBL height
250 250 250 using the Rig and Rib methods.

200 200 200


Z (m)

150 150 150

100 100 100

50 50 50

8 10 12 0 10 20 2 4
T ( oC ) Rig Rib

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Yuval, et al. Atmospheric Research 231 (2020) 104675

Fig. 4. Vertical profiles of the temperature, gradient Richardson


a b c number, Rig, and the bulk Richardson number, Rib, on 5 July 2014 at
350 350 350
01:31 (local time). A surface temperature inversion was not detected
and the PBL state was assigned to be an RBL, with its height de-
300 300 300 termined by the W&W and the bulk Richardson number methods (see
Fig. S3 in the Supplementary Material).
250 250 250

200 200 200


Z (m)

150 150 150

100 100 100

50 50 50

23 24 0 1 2 0 0.2 0.4
T ( oC ) Rig Rib

during the three PBL states between April and September are quite si- Table 3
milar. The median values of the cloud cover (okta), temperature (°C), the rate of
The monthly medians of the NOx and NO2 concentrations show surface temperature change in the five hours before launch time (∂T/∂t; ∘C
clear annual cycles in all PBL states, with highest values during winter h−1), relative humidity (%), wind speed (ms−1) and the standard deviation of
and lowest in summer. The annual cycle during SBL conditions is the the wind direction (StWD, degrees) during launch time for each of the three PBL
most prominent with concentrations during winter higher by factor of states. N is the minimal size of the variable samples for each PBL state.
4–5 compared to the summer. The NO concentrations are very low, N Cloud Cover Temp. ∂T/∂t RH Wind Speed StWd
virtually zero during RBL conditions, and during SBL conditions in
CBL 1431 2 27.3 0.82 51.7 4.1 17.6
March to September. In the case of CBL conditions (always daytime) the
RBL 426 4 23.0 −0.37 77.7 1.9 10.9
annual nitrogen oxides cycles can be partially explained by the higher SBL 1252 1 16.4 −0.68 82.3 1.4 6.9
summer solar radiation intensity and the resultant higher photo-
chemistry rates. However, at night-time (SBL and RBL conditions) this
explanation is not relevant and the character of the PBL may provide The monthly median O3 concentrations (Fig. 6e) during SBL con-
the answer. Certainly it is not the night-time PBL height that has causal ditions are very low with no annual cycle. Higher values with nega-
relationship with the concentrations of the primary pollutants since the tively correlated annual cycles are seen in the monthly median O3
correlations are positive (see Table S1). This is clearly demonstrated for curves during CBL and RBL conditions. This negative correlation points
SBL conditions, when the annual concentration cycles of all the primary to differences between CBL and RBL conditions in the O3 interaction
pollutants, PM2.5, NOx, NO2 and NO are very strongly positively cor- with locally produced NOx. O3 is a secondary pollutant with back-
related with the annual cycle of the SBL height (Table S1). That is, in ground concentrations of 45–60 ppb in Israel (higher in summer, lower
times of the year when the SBL is high, and presumably primary pol- in winter; Asaf et al., 2008). The daytime CBL O3 concentrations were
lutant concentrations should be low thanks to the large volume of the observed downwind from the main nitrogen oxides sources and the
atmosphere available for dispersion and mixing (Seinfeld and Pandis, daytime solar radiation is a strong determinant of their values, which
1998), their concentrations are actually high, and vice versa. On the are low in winter and high in summer. During SBL and RBL conditions
other hand, the annual cycle of the lapse rate during SBL conditions has (always night-time) the O3 concentrations are significantly lower,
a very strong negative correlation with the primary pollutant con- suggesting that their dominant determinant is titration of background
centrations (Table S1), pointing to the atmospheric stability during SBL O3 by the locally produced nitrogen oxides.
conditions as the most prominent, and probably the causative, factor in Figs. 5 and 6 show qualitative information about the seasonal trends
determining the primary pollutant concentrations. in the PBL characteristics and their impact on the seasonal variability of

Table 2
Descriptive statistics of PBL characteristics. The mean, standard deviation and percentiles were calculated for the samples of N valid values for each measure per each
PBL state. The PBL heights are given in metres. The lapse rate Γ, calculated using the 12th radiosonde record (24 s from launch, mean of 108 m), is in °C km−1.
Measure Method N Mean Std 5th 25th 50th 75th 95th

CBL hcblW W&W 1438 1013 624 287 531 865 1321 2345
hcblRb Rib 1426 1087 511 325 699 1049 1431 1987
hcblRb Rib 1426 1087 511 325 699 1049 1431 1987
Γ108 1438 21.8 10.8 8.6 14.0 20.4 28.4 41.0
RBL hrblW W&W 429 1216 657 333 711 1115 1609 2498
hrblRb Rib 404 248 292 0 50 129 352 892
Γ108 429 1.8 7.4 −10.8 −1.2 3.0 7.0 10.1
SBL hsblT Temp. 1256 122 72 42 64 108 160 266
hsblRg Rig 1131 102 59 23 57 89 138 215
hsblRb Rib 1072 34 69 0 4 15 33 128
Γ108 1256 −27.6 23.2 −71.7 −39.4 −20.8 −10.1 −3.1

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Yuval, et al. Atmospheric Research 231 (2020) 104675

a Fig. 5. Monthly median values of the PBL height


30 (continuous lines) and the lapse rate Γ (dashed
1350
lines). (a) CBL conditions; (b) RBL conditions; (c)
1200 25

( o C/km)
CBL (m)

SBL conditions. The PBL heights during CBL and RBL


1050 conditions were estimated using the W&W method.
20
900 The SBL height was estimated by the temperature
750 15 method. The lapse rate was calculated between the
600 temperature at the 12th radiosonde reporting level
10 data (24 s from launch, on average at 108 m) and the
Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec
second level (two seconds, on average 6.2 m.)
b
2100 6

1800

( o C/km)
RBL (m)

4
1500
1200 2
900
-0
Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec
c
0
140 -10

( o C/km)
SBL (m)

120 -20
100 -30
-40
80
-50
60
Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec

the pollutants. Table 4 provides corresponding quantitative measures of oxides concentrations, and negatively correlated with O3 concentra-
the associations at the daily time scale, with the seasonality in both tions. The correlations of the lapse rate with pollutant concentrations
pollution concentrations and PBL characteristics removed. The sea- during SBL conditions are always opposite in sign to those with the SBL
sonality was removed from the time series by constructing daily time height and are much larger in magnitude (by about 50%, with the ex-
series of the seasonal variation using spline interpolation of the monthly ception of the O3). The magnitudes of the SBL lapse rate correlations
medians shown in Fig. 5 and Fig. 6 and subtracting them from the with the concentrations of all the nitrogen oxides, the only pollutants of
original data series. The entries in Table 4 are the Spearman correlation which close to 100% are emitted locally in the study area, are sig-
coefficients between daily residuals of the pollutants at the times of the nificantly larger than the corresponding correlations with any other
radiosonde launches and the residuals of the corresponding PBL char- PBL characteristic for any PBL state. This attests to the prominence of
acteristics. Spearman correlation was used due to the asymmetric dis- the atmospheric stability in determining the concentrations of locally
tributions of some of the variables and the relatively small data samples emitted air pollutants.
in a few cases (e.g., RBL conditions). Only data from working days were Table S2 in the Supplementary Material shows the Spearman cor-
used in calculating the correlations in Table 4 to avoid bias due to the relation coefficients between daily values of pollutant concentrations
lower emissions in weekends and holidays. and the corresponding PBL characteristics without removal of the sea-
The correlations of the CBL height and of the daytime lapse rate sonal trends. Its results emphasise even more the finding in Table 4. We
with PM2.5 and nitrogen oxides concentrations are negative. This sup- believe though that considering the residuals, as in Table 4, promotes
ports the common view of the CBL as a mixing layer within which the additional insight about the association between the PBL characteristics
dispersion of locally produced pollutants occurs. It must be noted and the pollutant concentrations by eliminating the obvious effects of
though that the correlations are rather weak (< 0.5), with the magni- the seasonal variability (e.g., in solar radiation).
tude of the negative correlations of the CBL height estimated by the Rib The correlations shown for the whole study period in Table 4 vary
method somewhat larger compared to the corresponding correlations seasonally. Tables S3 and S4 show the winter and summer correlations
using the W&W method. The daytime lapse rate is only very weakly of the pollutants and the PBL characteristics, respectively. A few sub-
associated with the primary pollutant concentrations. The correlation stantial differences can be observed between the seasons, which can be
was also weak considering the lapse rate within the superadiabatic part summarised as (a) much stronger winter correlations between nitrogen
of the CBL (usually in between 20 and 100 m from the surface). The oxides concentrations and the CBL and RBL heights (especially con-
correlations of the O3 concentrations with all the daily PBL character- sidering the Rib method); (b) much stronger winter correlations be-
istics are positive but are very small in magnitude. The daytime O3 tween PM2.5 and O3 concentrations and the SBL heights; (c) much
concentration is probably determined mainly by the intensity of the stronger winter correlations of the pollutant concentrations (with the
solar radiation and the resultant photochemical reactions rates and less exception of O3) with the lapse rate during SBL conditions.
so by mechanical dispersion in the CBL. Table 4 presents the strength of the statistical association between
A more complicated picture is observed in the correlations of the pairs of PBL characteristic and air pollutant concentration series. This
pollutant concentrations with the night-time PBL characteristics. The analysis ignores the possible impact of additional variables that might
correlations of the RBL height with PM2.5 and nitrogen oxides con- be associated with both variables in each pair. Table 5 provides results
centrations are smaller in magnitude compared to the corresponding of multiple linear regression models where the impact of an explanatory
correlations during CBL conditions while the correlation with O3 are variable and its relative strength of association with the dependent
significantly higher, especially considering the RBL height using the Rib variable can be assessed while accounting for the impact of all the other
method. On the other hand, like with the correlations on the seasonal variables. The most dominant PBL characteristics, meteorological
scale, the SBL height is positively correlated with PM2.5 and nitrogen variables and the truck volume were used as explanatory variables to

7
Yuval, et al. Atmospheric Research 231 (2020) 104675

CBL
RBL
a SBL

g m -3 )
25

20

15

PM2.5 ( 10

b
50
NO x ( ppb )

40
30
20
10

c
30
NO 2 ( ppb )

20

10

d
15
NO ( ppb )

10

e
60
O3 ( ppb )

40

20

Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec

Fig. 6. Monthly median values of PM2.5, nitrogen oxides and O3 concentrations during CBL, RBL and SBL conditions.

Table 4
Spearman correlation between air pollutant concentrations and PBL characteristics at the daily time scale after removal of the seasonal variability.
CBL RBL SBL

hcblW hcblRb Γ108 hrblW hrblRb Γ108 hsblT hsblRg Γ108

PM2.5 −0.21 −0.18 −0.05 −0.16 −0.04 −0.02 0.18 0.13 −0.30
NOx −0.34 −0.43 −0.16 −0.31 −0.41 −0.49 0.38 0.37 −0.60
NO2 −0.36 −0.44 −0.18 −0.31 −0.41 −0.50 0.37 0.34 −0.58
NO −0.21 −0.30 −0.09 −0.03 −0.14 −0.13 0.32 0.31 −0.50
O3 0.05 0.15 0.03 0.24 0.45 0.26 −0.23 −0.30 0.28

estimate the NOx concentrations. Similar models were constructed also explanatory variables and the NOx concentration. Like in Table 4, the
for the other pollutants but the NOx, emitted almost exclusively by local seasonal cycles were removed from the data series. However, in this
sources, serves as the best example. The explanatory variable series case data from all days of the week, including the weekend, were used
were standardised (by removing the mean and division by the standard so that the impact of the NOx emissions (represented by the truck vo-
deviation) so the magnitude of the corresponding regression coeffi- lume) can be assessed. Table S5 provides the corresponding results
cients reflect the strength of the association between each of the using the original series without removal of the seasonal cycles. During

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Yuval, et al. Atmospheric Research 231 (2020) 104675

Table 5 and O3 concentrations during RBL and CBL conditions, their seasonal
Regression coefficients and their p–values (probability of the coefficient to be variability and their correlation with the RBL and CBL heights are very
sampled from a distribution with zero mean) of multiple linear regression different. As shown in Table 3 and in Fig. S5, the meteorological vari-
models estimating NOx concentrations using data from the whole study period. ables at times that RBL was detected are very different from those
The explanatory variable series were standardised so they are all non–dimen-
during either the CBL or SBL. Understanding them and the air pollutant
sional and range between zero and unity, with the coefficient magnitudes re-
concentrations which they bring about merits further examination in
flecting the relative contributions of the variables to the variance explained by
future when more data will be available.
the models.
We found the SBL height to be positively correlated with the con-
CBL RBL SBL centrations of primary pollutants at both the seasonal and daily time
scales (Table S1 and Table 4, respectively). This belies the perception of
Coeff. p-value coeff. p-value Coeff. p-value
the night-time PBL as a limiting volume in which pollutants can dis-
Γ108 −0.56 0.01 −5.61 < 0.001 −14.10 < 0.001 perse (e.g., Kotthaus et al., 2018). The negative and much stronger
Truck volume 2.08 < 0.001 0.27 0.46 4.68 < 0.001 correlation of the SBL lapse rate and primary pollutant concentrations
Solar radiation −0.58 0.003 NA NA NA NA
suggests that the causal relationship is of temperature gradients driving
Wind speed −2.00 < 0.001 −0.75 0.11 −4.15 < 0.001
PBL height −1.52 < 0.001 0.69 0.19 3.01 < 0.001 the significantly higher concentrations during SBL conditions. The po-
sitive correlation between the SBL height and the concentrations is most
probably just a confounding statistical association emerging because
daytime CBL conditions all the explanatory variables contribute sig- strong negative lapse rates promote large SBL thickness. Attesting to
nificantly to the regression model with large contributions of the wind that is the high negative correlation between the lapse rate and the SBL
speed, truck volume and the PBL height, and smaller contributions of height (around 0.6 after removal of their seasonality and 0.8 using the
the lapse rate and the solar radiation. During RBL conditions only the actual values). The strong negative temperature lapse rates during SBL
lapse rate seems an important determinant of the NOx concentrations. conditions suggest that the SBL in our area should not be considered a
On the other hand, during SBL conditions all the explanatory variables mixing layer as the very strong stability results in stratification and
contribute significantly to the NOx model but the contribution of the large vertical pollution concentration gradients even within the SBL.
lapse rate is by far the largest. It must be noted that the truck volume This finding is in agreement with results of model simulations carried
was available for us only as a mean value per day of the week and hour out by Taylor et al. (2014), and with the measurements of Han et al.
of the day. The impact of its actual daily variations is not accounted for (2009), Fig. 6) and Kwak et al. (2016), Fig. 5), which clearly show
and thus its relative contribution to the model should be regarded as an much higher concentrations of traffic–related primary pollutants near
underestimation. Notwithstanding, the very large regression coefficient the ground compared to their values aloft under such PBL conditions.
of the lapse rate during night-time (RBL and SBL conditions) most The temperature lapse rate during SBL conditions was found to be
probably reflects the prominence of the atmospheric stability in de- the PBL characteristic most strongly associated with air pollutant con-
termining the nocturnal NOx concentrations. centrations. We presented results of the lapse rate calculated from the
surface to the 12th radiosonde reporting level (24 s from launch, on
average at 108 m). As can be seen in Tables S6, S7 and S8, the lapse rate
4. Discussion and conclusions considering this level is not necessarily the one most strongly associated
with the air pollutant concentrations. The selection of this level was due
Five years of radiosonde records and corresponding air quality data to the fact that being close to the mean SBL height and the elevation of
were used to explore the associations between PBL characteristics and the CBL's superadiabatic sub–layer, the calculated lapse rate approxi-
pollutant concentrations. Unlike previous works, we studied these as- mately reflects the typically constant gradient of the temperature close
sociations while distinguishing between different PBL states. The to the surface. Our results suggest that the lapse rate is the appropriate
clearly lower concentrations of primary pollutants during CBL condi- parameter to consider while studying pollutant dispersion within the
tions, occurring in daytime when local emissions are high, emphasise PBL. The strength of its association with the pollutant concentrations
the importance of convective processes in determining pollutant con- depends on the nature of emission (areal/mobile sources or point ele-
centrations. However, unlike the common notion, the actual CBL height vated sources), and the type of pollutant (primary/secondary). We
is not a very strong determinant of the concentrations, especially in showed that at night–time (SBL and RBL conditions) the surface lapse
summer time, when in spite of the relatively low CBL height in the rate is strongly associated with concentrations of pollutants emitted at
study area (Fig. 5), its correlation with the pollutant concentrations is ground level. It should be noted that the surface lapse rate can be re-
very low (Table S4). latively cheaply and easily observed using two vertically spaced ther-
In a substantial number of the night-time records we did not detect mometers. Thus a simple setting of thermometers at the bottom and top
the classic nocturnal SBL, characterised by temperature increasing with of a water tower or a cellular microwave mast might provide in regions
height near the surface and topped by a low level inversion. In the similar to our study area more practically useful information regarding
majority of these cases a PBL top could be determined using the W&W pollution dispersion at night than costly remote sensing instruments or
and the Rib methods. We assumed these cases to be residual boundary radiosondes. The high correlation of the lapse rate measured from the
layers underneath which an SBL had yet to develop. This assumption surface to high elevations during daytime CBL conditions (Table S6)
was corroborated by their occurrence during cloudy nights with slow can be estimated by remote sensing or from meteorological model
cooling rate in the hours before the radiosonde launch. The high pre- output, and be used in statistical air pollution exposure models. Most
valence of RBLs during summer time (Fig. S4), when sunset and the propbably separated lapse rates within the CBL sub–layers should be
onset of SBL development occur at a later hour, also supports this as- considered for this purpose but understanding this issue is left for future
sumption. It is surprising though to find so many RBL cases given that studies.
even summer solstice sunset in the study area is at least 5–6 h prior to Many recent studies which used radiosonde data to determine the
the night-time radiosonde launch. The urban heat island of the Tel Aviv PBL height (Seidel et al., 2012; Guo et al., 2016; Liu et al., 2018; Miao
metropolitan area might be the reason. It would be interesting to et al., 2018) employed exclusively the Rib method, stating it is suitable
compare the results to a similar study carried out in a more rural set- for both stable and convective conditions. Following exactly the same
ting. The concentrations of nitrogen oxides during RBL conditions, and procedure for calculating the SBL height by the Rib method we found
their correlation with the RBL height, are similar to those of the day- that this method is not suitable for estimating the SBL height in our
time CBL and not to those of the night-time SBL. However, the PM2.5 study area. The SBL height determined by the Rib method was usually

9
Yuval, et al. Atmospheric Research 231 (2020) 104675

very low and in about 10% of the cases it indicated zero SBL height stably stratified turbulence. Atmospheric Science Letters 8, 65–69.
while a surface temperature inversion could clearly be observed. On the Grundström, M., Hak, C., Chen, D., Hallquist, M., Pleijel, H., 2015. Variation and co–v-
ariation of PM10, particle number concentration, NOx and NO2 in the urban air–
other hand, we found that the Rig method worked well and resulted in Relationships with wind speed, vertical temperature gradient and weather type.
SBL heights somewhat different but highly correlated with those found Atmos. Environ. 120, 317–327.
using the temperature method. During CBL and RBL conditions, we Guo, J., Miao, Y., Zhang, Y., Liu, H., Li, Z., Zhang, W., He, J., Lou, M., Yan, Y., Bian, L.,
Zhai, P., 2016. The climatology of planetary boundary layer height in China derived
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pollutant concentrations compared to using the W&W method. Our Han, S., Bian, H., Tie, X., Xie, Y., Sun, M., Liu, A., 2009. Impact of nocturnal planetary
results suggest that the Rib method is suitable for PBL height determi- boundary layer on urban air pollutants: Measurements from a 250-m tower over
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nation in unstable conditions but that care must be practised when it is Hennemuth, B., Lammert, A., 2006. Determination of the atmospheric boundary layer
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different instrumentation. A much smaller number of papers actually Kotthaus, S., Halios, C.H., Barlow, J.F., Grimmond, C.S.B., 2018. Volume for pollution
studied the association of the PBL height and air pollutant concentra- dispersion: London’s atmospheric boundary layer during ClearfLo observed with two
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Kwak, K.-H., Lee, S.-H., Seo, J.M., Park, S.-B., Baik, J.-J., 2016. Relationship between
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