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Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689

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Journal of Atmospheric and Solar-Terrestrial Physics


journal homepage: www.elsevier.com/locate/jastp

Meteorological factors affecting lower tropospheric ozone mixing


ratios in Bangkok, Thailand
S. Janjai a,n, S. Buntoung a, M. Nunez b, K. Chiwpreecha a, S. Pattarapanitchai a
a
Department of Physics, Faculty of Science, Silpakorn University, Nakhon Pathom 73000, Thailand
b
School of Land and Food, University of Tasmania, Hobart 7001, Australia

art ic l e i nf o a b s t r a c t

Article history: This paper examines the inuence of meteorological conditions in ozone mixing ratio measured at the
Received 4 March 2016 Thai Meteorological Department (TMD) in Bangkok, Thailand. In addition to surface wind speed and
Received in revised form direction, surface ozone concentrations, ozonesondes and CALIPSO Lidar images were collected during
28 June 2016
the study period extending from 01/01/2014 to 30/04/2015. Surface ozone concentrations show a strong
Accepted 6 July 2016
seasonality, with maximum in the dry months of December to April and minimum during the wet
Available online 7 July 2016
southwest (SW) monsoon period extending from May to October. High ozone concentrations are related
Keywords: to biomass burning in the northeast highland regions of the country and neighboring Myanmar and
Ozone mixing ratio southern China. These precursors travel in a southerly direction towards Bangkok in a well-dened
Ozonesonde
aerosol layer which may be at ground level or at elevated heights. The growth of the daytime mixed layer
Biomass burning
scavenges some of the upper level aerosols, although local maxima in ozone concentrations at 12 km
are a frequent feature at Bangkok. There is an evidence of fumigation in the Gulf of Thailand and a return
ow via the southerly sea breezes.
& 2016 Elsevier Ltd. All rights reserved.

1. Introduction Zhang and Kim Oanh (2002) found that local emissions and pho-
tochemistry are responsible for high ozone episodes and that high
Atmospheric ozone is an important factor in stratospheric ab- ozone levels were found downstream of the city centre, assuming
sorption of ultraviolet radiation (IPCC, 2007), but in the tropo- the northeast/east wind direction.
sphere it is a pollutant linked to a range of illnesses such as car- Despite the considerable progress made as outlined above,
diovascular diseases, strokes and respiratory problems (Zanobetti there is need for a better understanding of the basic wind ow and
et al., 2010). In southern Asia, a range of ozone precursors such as temperature structure associated with ozone concentrations.
motor vehicle emissions, industrial emissions and biomass burn- Measurements of ozone are a result of complex reactions involving
ing, combines to produce high levels of tropospheric ozone. Ty- photolytic source terms, as well as vertical and horizontal trans-
pically, the large megacity of Bangkok has levels of tropospheric port. In particular, there is need to assess the relative importance
ozone often exceeding the one hour standard (Zhang and Kim of the various precursor mechanisms which include local sources
Oanh, 2002; CAI-ASIA, 2009; Zhu et al., 2012). (industries, incinerator emissions, open res), mobile sources
Much of the research in southern Asia focuses on the re- (motor vehicles) and advective transport into the region from
lationship between high ozone concentrations and a range of en- biomass burning episodes located at a considerable distance up-
vironmental factors such as solar radiation and seasonal variability stream from Bangkok. Ideally a comprehensive measurement and
(Elampari and Chithambarathanu, 2011) and the photolytic cycle modelling programme would be required to accomplish these
(Nishanth and Kumar, 2011). Other studies use backward trajec- tasks, but it is beyond the scope of this study. As an alternative and
tory analysis with ozone measurements to study long-range as a preliminary study, we have chosen to examine measurements
transport of precursors released by biomass burning episodes, of ozone levels in the lower troposphere and relevant meteor-
these having been found to affect tropospheric and boundary layer ological factors at the Thai Meteorological Department (TMD) lo-
concentrations at considerable distances downstream (Sahu et al., cated in Bangkok. In the analysis, we examine ozone, air tem-
2013a, 2013b). Within the Bangkok Metropolitan Region (BMR), perature and wind speed proles at the site as well as surface O3,
NO2, CO and wind speed and direction. These data are also sup-
n
Corresponding author. plemented by Lidar backscatter images for the region, backward
E-mail address: serm.janjai@gmail.com (S. Janjai). trajectory analysis and satellite data on biomass burning.

http://dx.doi.org/10.1016/j.jastp.2016.07.008
1364-6826/& 2016 Elsevier Ltd. All rights reserved.
S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689 77

In Section 2 of this manuscript, we describe the site char- Table 1


acteristics, instrumentation and measurement programme. Sec- Estimating emissions of air pollutants for Bangkok in 1997. Source: PCD (2000), and
adapted from Zhang and Kim Oanh (2002).
tion 3 presents seasonal variation, and Section 4 discusses factors
relevant to ozone concentrations. Section 5 summarises the var- Pollutants Emission loads (tons/year)
ious meteorological factors involved in high O3 measurements at
the study site, and the conclusions are presented in Section 6. Point source Mobile source Area source Total

NOx 6553 164,737 6434 177,724


CO 909 249,320 4467 254,696
2. Methodology VOC 382 171,086 8468 179,936

2.1. Site characteristics


is associated with warm, humid and unstable air masses from the
The BMR encompasses Bangkok and ve surrounding provinces Indian Ocean and South China Sea from May to October. There is
including Samut Prakan, Nonthaburi, Pathumthani, Nakhon Pa- considerable precipitation during these months and an improve-
thom and Samut Sakhon (Fig. 1). It is located in the Chao Phraya ment in air quality compared to the winter months (Janjai et al.,
River Basin with a total area of 7762 km2 and with a population of 2014, 2015).
10.1 million (Zhu et al., 2012). The motor vehicle is a major source In this work, the study site is located at the TMD (13 39 58.57
of air pollution, although other sources such as power plants, in- N, 100 36 21.44 E, 2 m msl) in southern Bangkok (Fig. 1). It is
dustries, incinerators and biomass/residue burning also contribute surrounded by industries to the southeast and north, and several
to frequent episodes of poor air quality. Table 1 provides a source trafc highways.
inventory for the BMR, showing that volatile organic compound
(VOC) and Nitrogen oxides (NOx), two important ozone precursors, 2.2. Instrumentation and data acquisition
are mainly emitted from motor vehicles. However, sources trans-
ported into the region are not taken into account. The study encompassed the period 01/01/2014 to 30/04/2015.
The climate of the region is subject to the northeast (NE) Data collected are shown in Table 2. All meteorological and air
monsoon dominated by NE winds which extend from November quality data on-site with the exception of those collected with the
to February and which brings dry conditions, light winds and poor ozonesonde, were provided courtesy of the TMD and Pollution
air quality to these winter months. The southwest (SW) monsoon Control Department (PCD). The ozonesondes (Electrochemical

Fig. 1. Map of Thailand indicating the location of the study site which is located at the headquarter of the Thai Meteorological Department and the path of the CALIOP Lidar
instrument of CALIPSO, which are marked by dash line (daytime) and dot line (nighttime).
78
Table 2
Summary of all data collected for the study.

Instrument Variable Frequency Duration Accuracy

Surface analyzer instruments


Ultraviolet (UV) absorption photo- Surface O3 Continuous 01/01/2014-30/04/2015 o 0.5% of reading
metry instrument Continuous 01/01/2014-30/04/2015 0.5% of reading above 5 ppb

S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689
Chemiluminescence instrument Surface NO2 Continuous 01/01/2014-30/04/2015 0.5% of reading
Non-dispersive infrared detection Surface CO Continuous 01/01/2014-30/04/2015 0.5% of reading
instrument
UV-uorescence instrument Surface SO2
Sky radiometer (POM-01, SN: Aerosol optical depth at 500 nm Averaged daily 24/04/201430/04/2015 Wavelength accuracy: 2 nm
PS0825404) (daytime mean) Full opening view angle: 1 C
Operating temperature range:  10 to 45 C
Dobson spectrophotometer (BECK Total column ozone One daily (daytime 01/01/201430/04/2015 Ozone measurements with Dobson spectrophotometer No.90 were reliable within 13%
90) mean) of accuracy which quality assurance was undertaken by WMO SAG-Ozone on the Inter-
comparison in Tsukuba, 2006 and 2016.
Brewer spectrophotometer (MKIV) Total column ozone One daily (daytime 01/12/201417/03/2015 1% (for direct-sun total ozone)
mean)
Ozonesonde (ECC 2ZV7, EN-SCI Cor- Tropospheric ozone prole 1/month 2 days May 2014April 2015 1000 hPa, accuracy 5%
poration /Droplet Measurement of diurnal mea- 200 hPa, accuracy 12%
Technologies) surements (5) 100 hPa, accuracy 5%
10 hPa, accuracy 5%
4 hPa, accuracy 10%
Radiosonde (iMet-1-RSB 403 MHz Tropospheric wind speed, wind 1/month 2 days May 2014April 2015 Pressure, accuracy 0.5 hPa
GPS InterMet systems /Droplet direction, relative humidity and of diurnal mea- Temperature, accuracy 0.2 C
Measurement Technologies) air temperature surements (5) Relative humidity, accuracy 5%RH (  60 to 50 C)
Radisonde (RS92-DL, Vaisala) Tropospheric wind speed, wind 7:00 local time/ 01/01/201431/03/2015 Pressure, accuracy 1080-100 hPa: 1 hPa*
direction, relative humidity and day 100-3 hPa: 0.6 hPa*
air temperature Temperature, accuracy 0.5 C*
Relative humidity, accuracy 5%RH (  90 to 60 C)*
*2-sigma (k 2)
Anemometer (SIAP) Surface wind speed and wind 3 hourly 01/01/201430/04/2015 For wind speed, accuracy 1% or 0.2 m/s (0.25 to 50 m/s)
t031-TVV wind speed transducer direction For wind direction, accuracy 7 0.5
t033-TDV wind direction transducer
CALIPSO/CALIOP satellite Total backscatter attenuation at 15 good images 01/01/201430/04/2015 N/A
532 nm, displayed as images
OMI/AURA satellite Total column ozone One daily (daytime 01/01/201430/04/2015 Within 1% over the 30-year period of comparison, McPeters et al. (2015) (Comparison of
mean) OMI average ozone with the Brewer-Dobson networks)

Note: N/A means not being relevant.


S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689 79

concentration cell (ECC) model 2ZV7, EN-SCI Corporation/Droplet Ozone data from the UV absorption photometry instrument
Measurement Technologies) were used to measure ozone con- reacted strongly to solar radiation, and for processing purposes,
centrations up to a height of 37 km. Attached to the ozonesondes, surface ozone concentrations were integrated on a daily basis so as
radiosondes were also used to measure air relative humidity, air to give an average value between the hours of 09:00 and 15:00 LT.
temperature, total atmospheric pressure, wind velocity and wind The same procedure was followed for the sky radiometer data
direction. Sondes were released once monthly from May 2014 to which was only available for the period 23/04/2014 to 30/04/2015.
April 2015 with launch times at 09:00 local time (LT), two hours Wind speed and direction were processed at 07:00 and 16:00 LT
later than that of the radiosonde soundings taken by the TMD and averaged on a monthly basis. A total of 15 useful images were
(07:00 LT). Diurnal measurements were taken on 10/03/2015 and available after scanning all available data from CALIPSO/CALIOP.
07/04/2015. The main reason for the low number is that the ight/row path did

320

A
Total Column ozone (DU)

300

280

260

240
Dobson OMI Brewer ozonesonde
220
Aug-14

Oct-14
Nov-14
Jun-14
Feb-14

May-14

Jul-14

Sep-14

Feb-15

May-15
Apr-14

Dec-14

Apr-15
Mar-15
Jan-14

Mar-14

Jan-15
Date

90
Ozone concentration (ppbv)

80 B
70
60
50
40
30
20
10
0
Jun-14

Aug-14

Nov-14
Oct-14
Feb-14

May-14

Jul-14

Sep-14

Feb-15
Dec-14
Mar-14

Apr-14

Apr-15
Mar-15
Jan-14

Jan-15

Date

3.0
Aerosol optical depth at 500 nm

2.5
C
2.0

1.5

1.0

0.5

0.0
Mar-14

Oct-14

Mar-15
Jun-14

Aug-14

Nov-14

Jun-15
Feb-14

May-14

Jul-14

Sep-14

May-15
Apr-14

Dec-14

Apr-15
Jan-14

Jan-15

Date
Fig. 2. Seasonal daily variation of various quantities during the period 01/01/2014 to 31/05/2015 at the study site (13 39 58.57 N, 100 36 21.44 E): A) Daily column ozone
obtained from Dobson spectrophotometer, Brewer spectrophotometer, ozonesonde and OMI/AURA satellite; B) Daily average (09:0015:00 LT) surface ozone concentration
obtained from UV absorption photometry instrument; C) Daily average (09:00 15:00 LT) of aerosol optical depth at 500 nm obtained from the sky radiometer.
80 S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689

not coincide with Bangkok in most occasions. In addition, no Table 4


useful data were available during heavy cloudy periods and Percentage of wind direction frequency for the eight cardinal points at the study
site during 2014. A) 07:00 LT; B) 16:00 LT. Data exceeding 40% has been written in
especially in the wet monsoon season.
bold character.

Month N NE E SE S SW W NW Missing
3. Seasonal variation
A)
Jan 0 43 29 0 0 0 0 29 77
Fig. 2A shows daily total column ozone at the site with four Feb 0 43 0 0 57 0 0 0 75
different instruments. The satellite data is based on a daily pass Mar 0 0 0 20 80 0 0 0 52
(once a day) with a footprint of 13  24 km2 (http://aura.gsfc.nasa. Apr 0 20 0 0 67 0 7 0 50
May 0 0 7 0 82 9 9 0 64
gov/scinst/omi.html). Also shown are data when available from
Jun 0 0 0 0 18 18 64 0 61
surface Dobson and Brewer spectrophotometers and 10 selected Jul 0 0 10 0 45 45 0 0 64
days from the ozonesonde. There are differences between the Aug 0 0 7 0 36 36 21 0 55
Dobson spectrophotometer and Ozone Monitoring Instrument Sep 0 0 11 0 11 33 33 0 68
Oct 25 62 0 0 13 0 0 1 71
(OMI) data, especially in the SW summer monsoon which possibly
Nov 7 64 29 0 0 0 0 0 48
may be attributed to errors created by high relative humidity and Dec 9 82 0 0 0 0 0 0 64
high cloud cover affecting the inversion procedure of OMI. Despite
these small differences, all measurements support a marked sea-
B)
sonal variation in column ozone with a peak in mid-June and a Jan 0 44 6 6 31 12 0 1 45
minimum in mid-January. By contrast the daily average ozone Feb 0 14 8 12 54 12 0 0 7
concentration from the surface UV absorption photometer exhibits Mar 0 6 6 3 79 6 0 0 0
Apr 3 10 0 20 43 17 0 0 0
a very different seasonal pattern (Fig. 2B), with high values
May 0 0 0 0 74 26 0 7 0
(  50 ppbv) in the winter months (DecemberJanuary) and low Jun 0 0 0 4 60 36 0 0 20
values (  10 ppbv) in JulyAugust. These differences argue that for Jul 0 0 0 0 57 40 3 0 3
this site total column ozone is largely disconnected from tropo- Aug 0 0 0 0 29 57 7 7 3
spheric ozone, since the former is governed by surface emissions Sep 0 0 0 0 30 33 22 15 10
Oct 0 27 23 4 29 9 4 4 29
and boundary layer processes, while the later, column ozone is Nov 16 36 16 4 12 0 12 4 20
governed by features of the general circulation. Stratospheric Dec 4 39 15 8 15 11 0 8 16
ozone is a dominant component of total column ozone (Iqbal,
1983), so that variability in boundary layer ozone will not appear
or appear as a very weak signal in the estimate of column ozone.
As mentioned above, the seasonal pattern of surface ozone concentration for NO2 and O3 are large, with mean ozone levels
reacts to boundary layer processes with a maximum in winter being over four times larger and NO2 levels being over three times
months. This pattern is also very similar to the daily aerosol optical smaller in March compared to September.
depth at 500 nm obtained from the sky radiometer (Fig. 2C). These Seasonal wind direction data relates to transport of precursors
show a pronounced seasonal trend in aerosol optical depth (AOD), and these are given in Table 4A and B for 2014 at two times during
with minima around 0.1 in the SW monsoon months and maxima the day, in the morning (07:00 LT) and afternoon (16:00 LT). There
exceeding 1.0 in late March. In a later section, we will show that is a high frequency of calm winds at 07:00 LT which affects the
the AOD relates to transport of particulate matter from biomass percentage of missing data. Nevertheless both tables are con-
emissions which in turn act as precursors of ozone during high sistent in showing the marked seasonal shift in wind direction
ozone episodes. from the dry summer months dominated by easterly and north
Monthly statistics as measured by the surface analyzer for the easterly winds to the west monsoonal months dominated by the
main gas pollutants are shown in Table 3. Carbon monoxide (CO),
south westerlies. Highest frequency of NE winds occur during
nitrogen dioxide (NO2) and ozone (O3) exhibit seasonal variations
December for the morning observations (82%) and in January for
in their monthly averages with minimum concentrations in the
the afternoon observations (44%). Southwesterly wind directions
wet SW monsoon months and maximum in the dry months of
are most frequent in July for the morning observations (45%) and
January/December. By contrast no apparent trend is found for
in August for the afternoon observations (57%).
sulphur dioxide (SO2). Furthermore, the seasonal swing in
It is also of interest to examine the behavior of wind direction
inside the boundary layer in accordance with the objectives of this
Table 3
Mean monthly statistics from the surface analyzer of PCD installed at the study site study. To accomplish this, daily radiosonde soundings launched by
for the main anthropogenic gases. Numbers in brackets denote the 5 and 95 per- TMD were analysed. The data from the soundings were averaged
centile levels. over the bottom 3000 m and further averaged on a monthly basis.
Month CO (ppmv) SO2 (ppbv) NO2 (ppbv) O3 (ppbv) The results are shown in Table 5. There is a strong seasonal shift in
wind direction from the dry NE monsoon dominated by a north-
Jan-14 1.0 (2.0-0.2) 4 (8-2) 30 (79-7) 31 (82-2) erly component to the wet SW monsoon with winds from the
Feb-14 0.7 (2.3-0.1) 4 (7-2) 5 (22-0) 32 (52-10)
south. However both wind directions persist for all months, and in
Mar-14 0.5 (1.3-0.2) 5 (7-0) 3 (16-0) 32 (50-11)
Apr-14 0.7 (1.0-0.3) 2 (4-1) 7 (23-2) 26 (65-11) the height of the dry monsoon in December, 21 percent of direc-
May-14 0.5 (1.0-0.3) 3 (8-1) 11 (26-3) 17 (52-3) tions have a southerly component while 79 percent are from the
Jun-14 0.6 (1.0-0.3) 4 (8-1) 8 (18-2) 13 (31-1) north. Conversely in July 76 percent of components are from the
Jul-14 0.5 (1.0-0.5) 4 (11-2) 10 (18-1) 9 (30-2)
Aug-14 0.6 (1.3-0.0) 4 (10-2) 9 (18-1) 7 (35-1) south while 24 percent are from the north. High contamination
Sep-14 0.5 (0.9-0.1) 4 (9-1) 9 (18-4) 7 (40-1) episodes will occur in February to March and it is observed that
Oct-14 0.8 (1.7-0.4) 3 (6-20) 16 (38-4) 13 (65-1) this time of year is marked by a prevalence of winds from the
Nov-14 0.8 (1.7-0.3) 3 (7-0) 17 (44-4) 16 (64-3)
south (59 to 83 percent) but with a signicant percentage of winds
Dec-14 0.9 (1.8-0.3) 3 (6-0) 17 (43-3) 23 (65-2)
with a northerly component (17 to 41 percent, Table 5).
S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689 81

Table 5 measurements exceed 50 ppbv, these coming from the S and SW.
Percentage of the lowest 3000 m prole which is dominated by either a wind No signicant ozone transport occurs from other directions.
component from the north (NW, N, NE) or from the south (SW, S, SE). Wind di-
As expected, the low ozone concentrations during the wet
rection data used in this analysis were obtained from radiosonde sounding which is
daily launched by TMD for meteorological purpose. The data have been averaged season are consistent with the lack of any signicant precursors of
over all sounding taken in a particular month. Brackets denote standard deviations. ozone in the relatively clean air from the SW in addition to fre-
quent precipitation (Janjai et al., 2015). Biomass burning in the
Year Month Wind directions with a Wind directions with a south- north is a strong ozone precursor (Pochanart et al., 2001; Sonkaew
northerly component (%) erly component (%)
and Macatangay, 2015) which should enhance ozone concentra-
2014 Jan 79 ( 7 24) 21 (7 24) tions, and this observation is supported by Fig. 3A which shows
2014 Feb 26 ( 7 31) 74 ( 7 31) high ozone concentrations in a NE wind direction. An interesting
2014 Mar 17 ( 7 19) 83 ( 7 19) feature is the high concentrations coming from the southerly di-
2014 Apr 20 ( 7 17) 80 ( 7 17)
rection, implying a source of ozone in this direction or a re-cir-
2014 May 21 ( 7 25) 79 ( 7 25)
2014 Jun 19 ( 725) 81 ( 7 25) culation pattern. There are no known sources of ozone or its
2014 Jul 24 ( 733) 76 (7 33) precursor to the south in the Gulf of Thailand during the dry
2014 Aug 30 ( 7 28) 70 ( 7 28) months from February to April, so it is likely that these high
2014 Sep 55 ( 7 33) 45 ( 7 33) concentrations represent a re-circulation pattern.
2014 Oct 65 ( 7 31) 35 ( 7 31)
2014 Nov 68 ( 7 32) 32 ( 7 32)
Note that the transport from forest re in Indonesia was not
2014 Dec 79 ( 7 21) 21 (7 21) used for the explanation of the high ozone mixing ratios, because
2015 Jan 70 ( 7 30) 30 ( 7 30) this forest re occurs during May-October (Lestari et al., 2014;
2015 Feb 41 ( 7 40) 59 ( 7 40) Field and Shen, 2008) which does not correspond to the dry sea-
2015 Mar 33 ( 723) 67 ( 7 23)
son in Thailand.

4.2. Solar radiation and NO2 effects

4. Factors affecting surface ozone concentrations Solar radiation is an important factor in the photolytic cycle
and it is expected that surface ozone concentrations should show a
4.1. Wind direction strong sensitivity to it. To illustrate this process, we have selected
two monthly periods with the rst one extending from 01/12/2014
We next examine how surface ozone concentrations relate to to 31/01/2015, and the second one from 01/07/2014 to 31/08/2014.
wind direction, possibly indicating sources of ozone or its pre- Surface ozone, NO2 concentrations as well as global solar radiation
cursors. Concurrent three-hourly surface wind direction and ozone were averaged every hour and are presented (Fig. 4).
concentration data were selected, grouped and turned in polar There are several outstanding features in Fig. 4. Firstly, average
diagrams as shown in Fig. 3. solar radiation is very similar for these two time periods, differing
High ozone concentrations exceeding 75 ppbv occur with wind in their daily totals by 4%, with the July/August period being
directions predominantly from the NE and S in the dry season. slightly larger. In theory, July/August should be substantially
There is a much smaller component from the SW representing higher, having on average a lower noontime solar zenith angle
concentrations of around 1015%. Other concentrations are re- than in December/January. However cloud cover is larger in July/
presented to a much smaller degree. There are no concentrations August during the SW monsoon, so these two effects are likely to
exceeding 75 ppbv in the wet season and only 2% of equalise to give a similar pattern. Note that graphs in Fig. 4C

A N B N

W E

S S
Fig. 3. Diagram showing surface ozone concentrations and wind direction at the study site for A) Dry season (November 2014April 2015); B) Wet season (MayOctober,
2014). The color represents the concentration (ppbv). The radius distance indicates the percentage of the frequency of occurrence with respect to the total occurrence over
the season. The diagram is divided into eight sectors to indicate the wind direction.
82 S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689

100
90 Dec 2014 - Jan 2015 NO2
NO2
A O3
O3
80

Concentration (ppbv)
70
60
50
40
30
20
10
0
0 2 4 6 8 10 12 14 16 18 20 22 24

Hour (LT)

35
B Jul - Aug, 2014 NO2
NO2
30 O3
O3
Concentration (ppbv)

25

20

15

10

0
0 2 4 6 8 10 12 14 16 18 20 22 24
Hour (LT)

3.5
C Dec 2014 - Jan 2015
Global solar radiation (MJ/m^2)

3.0
Jul - Aug, 2014
2.5

2.0

1.5

1.0

0.5

0.0
5 7 9 11 13 15 17 19
Hour (LT)
Fig. 4. Hourly averages of A) surface ozone and NO2 concentrations during December 2014 and January 2015; B) surface ozone and NO2 concentrations during JulyAugust,
2014; C) hourly global solar radiation for the periods December 2014 and January 2015; and JulyAugust 2014.

represents the diurnal variation of monthly average hourly radia- to a later time, around 15:00 LT in July/August and 16:00 LT in
tion, thus smoothing out local irregularities that appear randomly December/January.
during the day. Ozone concentrations in both time periods react to Ozone concentrations in the boundary layer represent a bal-
solar radiation, but the December/January concentrations are ance between generation and destruction processes. Most im-
much larger, indicating a more active photolytic cycle which reacts portant is the photolytic cycle (Crutzen, 1995; Seinfeld and Pandis,
to available precursors. Furthermore, peaks in concentration are 2006) where ozone production is generated by the photo-
not reached at solar noon, approximately 12:00 LT but are shifted dissociation of NO2 and destroyed by titration of NO. Under steady
S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689 83

3.5 concentrations at 3 km exceed this value. A seasonal variation in


21-May Wet season A peak concentrations is suggested in Fig. 5A, with May, June and
13-Jun
3.0 July recovering from the dry season exhibiting highest levels, fol-
15-Jul
lowed by the lowest peaks in the main SW monsoon months of
8-Aug
2.5 August and September and increasing again in October. The dry
10-Sep
season proles (Fig. 5B) show increasing peak concentrations as
28-Oct
Altitude (km)

2.0 the dry season progresses. Highest levels are reached on 10/03/
2015 with concentrations of 75 ppbv at 2 km. These levels are
1.5 signicantly higher than in the wet season.
Ojha et al. (2014) using weekly ozonesondes also report a tro-
pospheric maximum in Nainital, in the Indian Himalayas, of
1.0
96 ppbv which they attribute to localised res in the spring
months in combination with other sources of regional pollution.
0.5
Using trajectory analysis in combination with surface ozone
measurements at two sites in India, Pochanart et al. (2001) relate
0.0
0 10 20 30 40 50
the W/NW trajectories to high O3 mixing ratios, reaching max-
imum levels of 70 ppbv in the summer months of March and April.
Ozone mixing ratio (ppbv)
They attribute to forest res and agricultural waste burning in the
3.5 South China-Myanmar-Thailand providing the needed precursors.
25-Nov Dry season B Our measurements support these ndings and we argue that up-
3.0
9-Dec per level tropospheric transport from the northern highlands is an
20-Jan important mechanism of ozone production in Bangkok. Ad-
20-Feb ditionally, an elevated transport above the localised boundary
2.5
10-Mar layer would minimise the downward ux of ozone (Matsuda et al.,
Altitude (km)

7-Apr 2005), therefore increasing the transport efciency and range and
2.0
allowing ozone mixing ratios or its precursors to reach other re-
gions of the Asian continent (Yonemura et al., 2002; Liu et al.,
1.5
1999).
Diurnal variations are next examined for the two measurement
1.0 days on 10/03/2015 and 07/04/2015 (Fig. 6 and Table 6). Both days
show a general increase in the integrated mixing ratio as the day
0.5 progresses from early morning (06:00) to late afternoon (16:00).
In March the column ozone (04 km) changed from 20.8 to 24.7
0.0 DU, an increase of 18.9% while in April the column ozone change
0 10 20 30 40 50 60 70 80
was 25.2%. Increases may relate to photolytic reactions at the
Ozone mixing ratio (ppbv) surface and downward transport of O3 from upper levels which are
Fig. 5. Ozone soundings showing mixing ratios in the bottom 3000 m of the at- also undergoing photolytic reactions. Peak concentrations for both
mosphere for A) the wet season from May-October, 2014 and B) the dry season days exhibit maximum values at 16:00 LT.
from November 2014 to April 2015. Circles denote localised maxima. Proles of potential air temperature and altitude were next
examined on 10/03/2015 and 07/04/2015, the two days with
state conditions, these two processes balance, although precursors diurnal measurements (Fig. 7). The effect of daytime sensible
such as NOx, CO, non-methane hydrocarbons (NMHC) excersise an heating may be seen as a sharp boundary between a vertical line
important role (Jeelani, 2014), shifting the balance either way. indicating neutral conditions and the overlying stable lapse rate
Hourly NO2 concentrations are presented in Fig. 4A and B which (Stull, 1988). In 10/03/2015, these occur at 700 m (09:00), 600 m
trend in opposite direction to the ozone concentrations, indicating (16:00) and 350 m (20:00), while on 07/04/2015, they occur at
an active role in photodissociation and production of O3 and in 500 m (06:00), 750 m (13:00) and 400 m (16:00). No neutral layer
agreement with the published literature (Sahu and Saxena, 2015; was encountered on 07/04/2015 at 06:00.
Sahu et al., 2016; Katragkou et al., 2015; Jeelani, 2014). Similarly, a There is no evidence that the mixing layer reached 1000 m or
post-noon peak in O3 is a consistent feature that has previously above where these peak concentrations were found. Nevertheless
been documented (Katragkou et al., 2015; Jeelani, 2014). it is reasonable to expect that some of these high ozone con-
centrations below 1000 m would be mixed and transported
4.3. Vertical transport and diffusion of ozone and temperature downwards as the neutral boundary layer grows during the day
(Fig. 7B). Unfortunately this process could not be clearly seen given
We next examine upper level processes to determine their in- the low number of ozone soundings per day available.
uences on surface ozone concentrations, and in particular their
vertical transport. Proles of ozone mixing ratio taken with the 4.4. Long-range transport
ozonesonde in the bottom 3000 m of the atmosphere are shown in
Fig. 5, with data being grouped into wet season, Fig. 5A and dry Data from the polar-orbiting Cloud-Aerosol Lidar and Infrared
season, Fig. 5B. As discussed earlier, all soundings with the ex- Pathnder Satellite Observations (CALIPSO) and specically ima-
ception of 10/03/2015 and 07/04/2015 were launched at 09:00 LT. ges from the Calibrated Lidar Prole CAL_LID_L1-VALTAGE1-V3-30
Both Fig. 5A and B exhibit distinct peaks in the maxima which (www.calipso.larc.nasa.gov) were acquired. These were examined
we dene as the level with the highest concentration in the for evidence of an aerosol cloud layer above the region, its char-
3000 m layer and at the same time exhibit a localised maximum acteristics, movement, enhancement or demise. We have used the
concentration. Using this denition, localised maxima are found total attenuated backscattered signal at 532 nm with a footprint of
with the exception of 08/08/2014 which does not exhibit a max- 300 nm and vertical resolution of 3060 m (Winker et al., 2007) as
imum and 28/10/ 2014 which has a local maximum at 1.3 km but providing most information. The instrument samples globally with
84 S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689

4.0 4000
10/03/2015 0600 A 6:00 10/03/2015
3.5 10/03/2015 0900 3500 9:00
10/03/2015 1600 16:00
3.0 10/03/2015 2000
3000 20:00

2500

Altitude (m)
2.5
Altitude (km)

2.0 2000

1.5 1500

1000
1.0

500
0.5 A
0
0.0 295 300 305 310 315 320
0 20 40 60 80 100
ozone mixing ratio (ppbv) Potential temperature (K)

4000
4.0 6:00 07/04/2015
07/04/2015 0600 B 3500 13:00
3.5 07/04/2015 1300 16:00
07/04/2015 1600
3000
3.0
2500
2.5 Altitude (m)
Altitude (km)

2000
2.0
1500
1.5
1000
1.0
500
0.5 B
0
0.0 295 300 305 310 315 320
0 20 40 60 80 100
Potential temperature (K)
ozone mixing ratio (ppbv)
Fig. 7. Potential temperature proles taken with the ozonesonde on A) 10/03/2015
Fig. 6. Diurnal ozone mixing ratios taken on A) 10/03/2015 and B) 07/04/2015 and B) 07/04/2015. Arrows indicate the altitude of the mixing layer.
Circle denote peak concentrations.

Table 6 02/01/2014 the backscatter signal appears to originate at around


Peak concentration (ppbv) and total column ozone (DU) in the bottom layer 04 km 20N, 99E and with concentrations evenly distributed in the rst
for March 10 and April 7, 2015. 2 km. The same northern emissions appears on the 10/03/2015,
with the exception that concentrations are elevated and show only
Time (LT)
a relatively small downward displacement. Downward transport
06:00 09:00 13:00 16:00 20:00 from the upper layers to the surface (fumigation) may occur as
shown in Fig. 8C and D. There is an elevated high concentration
March 10 Peak mixing ratio (ppbv) 72.7 75.0 99.0 78.1 layer in the daytime image (21/01/2015 at 13:53 LT) but approxi-
Total column ozone, 04 km 20.8 21.0 24.7 22.0
(DU)
mately 12 hours later concentrations are evenly mixed in the
bottom 2 km (Fig. 8D). This change is likely to result from further
growth of the daytime boundary layer in the afternoon and
April 7 Peak mixing ratio (ppbv) 67.4 74.2 85.3
Total column ozone, 04 km 18.9 22.2 23.7
scavenging of the upper concentrations. Other fumigation events
(DU) originate downstream over water in the Gulf of Thailand, possibly
related to a different stability environment. Red arrows in as such
Fig. 8EG show locations where concentrations have reached the
a visit to the Bangkok region (13.51N to 14.0N; 100.27E to surface.
100.92E) twice a month. Each cloud-free image was examined
and visual information on base and top height of the aerosol layer 4.5. The sea breeze as a return ow mechanism
was determined as well as the height of maximum backscatter
(Table 7). Southerly winds with their February onset (Tables 4 and 5) are
The 15 useful images retrieved show a distinct aerosol layer attributed to sea breeze effects initiated by differential heating of the
extending from 0.3 to 3 km (Fig. 8). The path/row orientation of ground as the land progressively warms above oceanic temperatures
the satellite path is in a NW/SE direction during the day and all in the Thai dry season (Phan and Manomaiphiboon, 2012; Janjai
images clearly show the aerosol originating in the highlands of the et al., 2014). These published studies indicate that the sea breeze may
NE of the country and transported in a southerly direction by re- penetrate to a maximum of 50 km and are weak and shallow. As
gional winds. As an example we show two images taken on 02/01/ such they can act as a return ow mechanism. Concentrations that
2014 and 10/03/2015 that illustrate this effect (Fig. 8A, B). On the have been brought down to the surface by fumigation or other
S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689 85

Table 7
Aerosol physical characteristics determined from total attenuated backscatter at 532 nm from CALIPSO/Lidar image. Data presented cover all suitable images during the
study period 01/01/201430/04/2015.

Date Time (UTC) Base height (km) Top height (km) Layer thickness (km)

02/01/2014 06:45:3006:58:59 0 1 1
18/01/2014 06:46:4807:00:17 0 2 2
19/02/2014 06:49:2007:02:49 0 0.3 0.3
07/03/2014 06:51:3107:05:00 0.5 2.5 2
23/03/2014 06:53:3707:07:06 0 1.5 1.5
08/04/2014 06:42:0006:55:28 0 3 3
18/11/2014 06:46:5407:00:23 0 2 2
20/12/2014 06:45:3106:59:00 0.5 1.5 1
20/12/2014 18:57:1319:10:42 0 1 1
05/01/2015 06:46:0706:59:36 0 2 2
21/01/2015 06:46:5807:00:27 0 2 2
21/01/2015 18:58:1419:11:43 0 2.5 2.5
06/02/2015 18:59:5619:13:25 0 2 2
10/03/2015 06:52:1507:05:44 0.5 2 1.5
11/04/2015 06:42:1606:55:45 0 1.5 1.5

Fig. 8. Proles of total attenuated backscatter at 532 nm from the CALIOP Lidar instrument of CALIPSO. In the daytime (13:00-14:00 LT), they cover a NW/SE swath while at
nighttime (01:0002:00 LT) they are from the SW/NE. All images, with the exception of Fig. 8G include Bangkok, which are marked by red rectangle.

processes (Fig. 8EG) may be transported back to Bangkok by the sea Further evidence on the vertical structure may be seen in
breeze, feeding the photolytic cycle with added precursors. This Fig. 9A and B which show the ozonesonde wind directions at
process can also explain the high ozone mixing ratios found for various times of the day. Both diagrams feature a well-dened
southerly winds during the dry season, Fig. 3A. wind direction from the S/SW in the bottom 1 km for all
86 S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689

3.5 from January to April and involve emission of ozone precursors,


10/03/2015 6:00
mainly NMHC and CO. They are released in the highland areas of
9:00
3 16:00
northern Thailand, Myanmar, Laos, Southern China and Vietnam
20:00 where they are transported southward by the prevailing N winds
(Fig. A and B). Depending on the stability of the atmosphere and
2.5
local dynamic ow, the emissions will stay at the upper levels
during its southward journey or proceed at ground level as a
Altitude (km)

2 mixed aerosol and cloud with typical thickness of 12 km. These


precursors enhance the urban photolytic cycle of Bangkok, raising
1.5
O3 concentrations during the dry months before the SW monsoon.

2) Vertical transport and diffusion


1

For surface-level ow, there is loss to the surface from turbu-


Northerly 0.5 Southerly lent ux, and maximum deposition velocities of 0.7 cm s  1 have
component component been measured in Teak forests in northern Thailand during the dry
season (Matsuda et al., 2005). For upper level ow, there is en-
0
0 60 120 180 240 300 360 trainment of precursor concentrations by the growing mixed layer
Wind direction (degrees) during the daytime (Stull, 1988; Seinfeld and Pandis, 2006; Lyons
and Cole, 1976), although our measurements indicate that the
3.5 mixed layer will not reach a considerable number of high altitude
07/04/2015 6:00
concentrations (Fig. 10A and B). There may also be additional fu-
13:00
3 migation as the upper level aerosol and cloud reaches the Bangkok
16:00
boundary layer, encountering an increasingly unstable atmosphere
2.5 (Oke, 1987, 1988 and Fig. 10A and B). At night vertical diffusion is
dampened and entrainment is no longer active.
Altitude (km)

2
3) Fumigation and re-circulation

1.5
Upper levels concentrations may be mixed downstream from
Bangkok, in the Gulf of Thailand as the air mass encounters a
1 different stability regime. The aerosol layer in one occasion at
night, Fig. 8G, appeared to show very little mixing during its
0.5 downstream trajectory which missed Bangkok until nally im-
Northerly Southerly pacting on the Gulf of Thailand. These surface concentrations are
component component
0 then re-circulated back into Bangkok by the sea breeze (Fig. 10B)
-180 -120 -60 0 60 120 180 240 300 360 during the day, increasing surface concentrations during February
Wind direction (degree) to April until rain events are encountered and/or biomass burning
ceases. It is also likely that O3 concentrations from the sea breeze
Fig. 9. Wind directions vs altitude for A) 10/03/2015 and B) 07/04/2015. Each graph
represents the data from of our radiosonde which was attached to the ozonesonde will be subject to other transport mechanisms unique to the urban
launched at the time indicated in the gures. regional climate of Bangkok in a similar fashion to those reported
for other cities (Hidalgo et al., 2008; Lemonsu et al., 2004; Lem-
onsu and Masson, 2002, Oke, 1987, 1988).
soundings, followed by a transition zone and a return ow above
with a northerly wind component. On the 10/03/2015 winds di-
4) Relative importance of precursor mechanisms
rections from the NE/E prevailed above 2 km, while on the 07/04/
2015, a NW ow appeared at 13:00 between 1.0 to 1.5 km and
A rough estimate of the importance of various mechanisms in
easterly winds featured for all soundings above 1.5 km.
high ozone episodes may be estimated using multiple linear re-
gression analysis. We have taken daily surface ozone recorded at
the study site as the dependent variable and measured NO2, CO,
5. Summary of meteorological processes affecting episodes of
aerosol optical depth (AOD) and solar radiation (RAD) as in-
high ozone concentration at the study site
dependent variables. All measured gases from the analyser were
averaged on a daily basis between 23/04/2014 and 30/04/2015, a
Given the various data sources examined in this study, it is
period with available data for all variables. Hourly values of solar
possible to outline the most important mechanisms involved in
radiation were summed to arrive at a daily value, also for the same
the transport and diffusion of ozone and its precursors. The dis-
time period. The regression using all available data of this period
cussion is arranged in temporal sequence following the generation
had the form:
of ozone and its development (see also Fig. 10).
O3 = 7.20491 + 11.947AOD + 0.4389NO2 + 0.893RAD
1) Sources (1)
+ 4.728CO
2
Forest res and agricultural burning of waste products from R 0.286; n 230 where NO2 (ppbv); CO (ppmv); AOD (unit-
crop production are believed to be the main sources of ozone less) and RAD (MJ/m2).
precursors (Crutzen et al., 1985; Liu et al., 1999; Pochanart et al., Our procedure estimates what percentage of the variance is
2001; Zhang and Kim Oanh, 2002; Sonkaew and Macatangay, explained with all variables and with one variable removed. The
2015). These biomass burning activities start during the dry period relative importance of each variable is assessed by its ability to
S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689 87

Fig. 10. Schematic showing likely transport and re-circulation of biomass burning in the region for nighttime (A) and daytime conditions (B).

Table 8 months from December 2014 to March 2015 inclusive. In de-


Regression analysis between O3 (dependent variable) and independent variables creasing order of importance, NO2, AOD contribute to the variance,
aerosol optical depth (AOD), nitrogen dioxide (NO2), carbon monoxide (CO), and
but CO, SO2 and radiation offer very little explanation. As expected
solar radiation (RAD).
solar radiation does not vary during the summer months and the
Total sum of Regression sum of Percent decrease in re- degree of explanation is minimal. It is however important to note
squares squares gression sum of squares that the analysis refers to high O3 episodes in the dry season. In
the absence of biomass precursors, local emissions from motor
All variables 21,670.2 6460.7
Minus AOD 21,670.2 2453.0 62.0
vehicles and industries become important (Zhang and Kim Oanh,
Minus RAD 21,670.2 4340.0 32.8 2002).
Minus NO2 21,670.2 4806.8 25.6 Monthly aerosol optical depth measured at the site is well re-
Minus CO 21,670.2 6114.0 5.4 lated to the total number of hot spots as obtained from satellite
data estimated for Thailand and neighbouring countries (http://
asmc.asean.org). Fig. 11 shows that the relationship between the
explain some of the variance in the regression (Judd et al., 2008). two variables is well dened during the dry months, although
Table 8 shows the results. more data needs to be acquired to establish a stronger
In order of importance, AOD is highest in explaining the O3 relationship.
variability, followed by solar radiation, NO2 and CO. Similar results Examination of back trajectories using NOAA HYSPLIT data
are obtained when the test was repeated for the dry summer (Stein et al., 2015) for the 12 days of ozonesondes revealed air
88 S. Janjai et al. / Journal of Atmospheric and Solar-Terrestrial Physics 147 (2016) 7689

0.8 from motor vehicles. Re-circulation from sea breeze events are
also likely to play an important part.
Average O3 concentrations (ppbv)

0.7
2) A distinct seasonal variation was found in daily surface ozone
0.6 concentrations and aerosol optical depth, with maximum values
0.5 in the dry season November to April and minimum values in the
wet season May to October inclusive.
0.4
3) Wind rose analysis, back trajectory analysis and Calipso images
0.3 provide information on the relevant mechanisms for high con-
centration episodes. Precursors originate in the northern re-
0.2
Jun-Nov
May-Oct gions of the country or in neighbouring Myanmar, China, Laos
0.1 and Vietnam as a result of biomass burning.
Dec-May
Nov-Apr
0 4) Particulate and gaseous emissions from biomass burning are
0 5000 10000 15000 20000 25000 30000 transported in a southerly direction by regional winds as ele-
Total number of hot spots vated plumes above the boundary layer or as mixed aerosols
Fig. 11. Graph of total number of hot spots per month vs average ozone con- within the boundary layer.
centrations at the study site. Hot spots have been summed over Thailand, Cam- 5) Some upper air concentrations are transported downward by
bodia, Myanmar and Laos. the growing neutral/unstable boundary layer during the day
over Bangkok.
6) Concentrations that have been brought down to the surface by
fumigation or other processes in the Gulf of Thailand (Fig. 8EG)
may be transported back to Bangkok by the sea breeze, feeding
the photolytic cycle with added precursors.

In conclusion, it must be emphasised that the work is pre-


liminary in nature and there is need for a more comprehensive
program to fully understand the relevant transport processes in
the Bangkok region. This must involve, for example a compre-
hensive wind measurement programme coupled with additional
surface ozone concentrations and ozonesonde measurements.
Future studies such as these will help understand how biomass
burning affects ozone levels in Bangkok and its potential impact
on human health and on the Bangkok ecosystem.

Acknowledgements

The author would like to thank the Silpakorn University Re-


Fig. 12. A typical back trajectory from HYSPLIT at the altitude of 1000 m on 25/11/ search and Development Institute to provide a research grant to
2014 (07:00 LT). (The vertical axis represents the latitude of the location, the hor- this project and to the Thailand Research Fund (TRF) for partially
izontal axis denotes the longitude of the location and the black star indicates the support of the project through the International Research Network
study site).
(IRN). We also thank the Thai Meteorological Department (TMD)
for the technical support in launching the ozonesondes and for
mass sources in the Indian Ocean for the SW monsoon days: 21/ providing aerosol, radiation and meteorological data. The Pollution
05/2014, 13/06/2014, 15/07/2014, 08/08/2014, 10/09/2014. During Control Department (PCD) is gratefully acknowledged for provid-
the drier periods NE winds dominate in four out of the seven days ing ozone and other related data for this work.
(28/10/2014, 25/11/2014, 09/12/2014, 20/01/2016) and over a 24 h
backward trajectory the ows are generally close to the Thai/
Cambodian border, therefore conrming our hypothesis regarding
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