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Journal of Atmospheric and Solar-Terrestrial Physics 182 (2019) 165–176

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Journal of Atmospheric and Solar-Terrestrial Physics


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

Characterizing black carbon aerosols in relation to atmospheric boundary T


layer height during wet removal processes over a semi urban location
M. Ashok Williamsa, T.V. Lakshmi Kumara,∗, D. Narayana Raob
a
Atmospheric Science Research Laboratory, Dept of Physics, SRM Institute of Science and Technology, Kattankulathur, India
b
SRM Institute of Science and Technology, Kattankulathur, India

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

Keywords: Black Carbon (BC) mass concentration has been analysed during rainy and non-rainy days of Northeast (NE)
Black carbon aerosols Monsoon months of the years 2015 and 2017 over a semi-urban environment near Chennai (12.81 N, 80.03 E),
Boundary layer height and wet removal located on the east coast of India. BC, measured using an Aethalometer (AE-31) has been related to the atmo-
processes spheric Boundary Layer Height (BLH) obtained from the ERA Interim Reanalysis data during rainy and non-rainy
days on monthly mean basis to understand the wet removal of BC over the study location. The study reveals that
BLH has a profound effect on the BC concentration on rainy days and non rainy days. It is found that the BC
concentration in the night time is lower on rainy days compared to non rainy days owing to wash out on rainy
days and the BLH remaining nearly the same on rainy and non rainy days. On the other hand, in the daytime it is
found that the BC concentration remains nearly the same on rainy and non rainy days whereas the BLH is lower
on rainy days compared to non rainy days. This reveals that in daytime lower boundary layer heights com-
pensate for the wet removal effect on BC concentration on rainy days. A quantitative relation is found between
the product of BC and BLH during rainy and non-rainy days which indicates the extent of redistribution of BC
during non-rainy days when compared to the rainy days. In the process of analysing BC during the wet removal
processes, the basic features of BC such as its mean diurnal variations, transport pathways, local sources and its
relation with relative humidity were also reported.

1. Introduction increased convective mixing within the atmospheric boundary layer.


Aruna et al. (2016) found the mass fraction of BC with PM10 during the
Black Carbon aerosols absorb the incoming solar radiation and year 2013 over Chennai is high during the south west monsoon (June to
cause positive radiative forcing in the atmosphere. The characteristics September) though they are quite less in magnitude. Using the BC
of black carbon aerosols such as their absorption, sources and their measurements from an aethalometer (AE 31) at Wuhan University in
transport in the Indian region have been discussed and well docu- China, Liu et al. (2018) found that BC mass concentration suppresses
mented by numerous researchers (Nair et al., 2007; Ramachandran and the BLH during the polluted days which in turn lead to poor air quality.
Kedia, 2010; Suresh Kumar Reddy et al., 2012; Rajeevan et al., 2018). Though there are many studies as mentioned earlier to characterise the
The main findings of the studies include the dependence of black black carbon aerosols, studies on their variations during rainy days are
carbon aerosol concentration on Atmospheric BLH (Babu and Moorthy, rather sparse. It is known that aerosols are removed from the atmo-
2002; Aruna et al., 2013), and association with synoptic meteorological sphere due to rain (Ramachandran, 2017). Aerosols which act as cloud
conditions (Babu and Moorthy, 2002; Tripathi et al., 2005; condensation nuclei (CCN) are removed by the process of rainout.
Udayasoorian et al., 2014). It is reported that BC maintains the diurnal Aerosols, mainly black carbon that may not be effective as CCN, are
and seasonal variations and are strongly linked to the atmospheric removed by the wash out processes. It is reported that 90–95% of the
boundary layer dynamics (Babu and Moorthy, 2002). Beegum et al. aerosols in the atmosphere are removed by the nucleation process (rain
(2009) studied the BC variations over different locations of India and out) and the remaining 5–10% of the aerosols, where BC mainly con-
reported that BC is high in mainland stations compared to highland tributes are removed by the impaction method (wash out) (Croft et al.,
stations during the premonsoon season (March to May). They also 2010). Studies exist to examine the BC levels in the rain water and
found that BC showed decreasing tendency in some stations due to the further to estimate the BC scavenging fluxes which are very much


Corresponding author.
E-mail address: lkumarap@hotmail.com (T.V.L. Kumar).

https://doi.org/10.1016/j.jastp.2018.11.018
Received 15 April 2018; Received in revised form 27 November 2018; Accepted 29 November 2018
Available online 30 November 2018
1364-6826/ © 2018 Elsevier Ltd. All rights reserved.
M.A. Williams et al. Journal of Atmospheric and Solar-Terrestrial Physics 182 (2019) 165–176

Fig. 1. Mean diurnal variation of BC mass concentration (μg/m3) for the study period (Oct–Dec 2015 and Oct–Nov 2017).

Fig. 2. (a & b). 3- day cluster mean trajectories arriving the site during a) Oct–Dec 2015 and b) Oct–Nov 2017

important to understand the BC life cycle in the atmosphere (Torres m3 BC reduction takes place.
et al., 2014; Taylor et al., 2014; Budhavant et al., 2016). Based on the In view of the dependence of BC on BLH, it would be interesting to
campaign conducted during the Integrated Campaign for Aerosols, study the effect of the wash out process on the dependence of BC on
gases and Radiation Budget (ICARB) experiment over Chennai, Suresh BLH. The present study portrays the changes in the BC mass con-
Babu et al. (2010) reported that the actual black carbon mass con- centration levels during rainy and non-rainy days of North East mon-
centration exhibits the longitudinal fluctuations within the marine soon (October to December) of 2015 and October and November of
boundary layer (below 500 m) and almost steady above the marine 2017 on a monthly mean basis over a semi urban location (SRM IST;
boundary layer heights (above 1500 m) over the different locations of 12.81 N, 80.03 E) of Chennai. The study location experienced severe
Chennai and nearby off shore locations. Cape et al. (2012) studied the floods during the November and December months of 2015 due to the
life time of BC using the emissions from the diesel engine vehicles over excessive amounts of rainfall (IMD, 2016). The diurnal changes in BC
a rural location in Scotland and found the life time of BC varies from 4 have been studied in relation to the changes in the BLH over this lo-
to 12 days. Madhavi Latha et al., 2005 studied the scavenging efficiency cation during rainy and non-rainy days along with the changes in air
of rainfall on BC over an urban environment of Hyderabad and reported temperature to understand the wet removal processes of BC over the
that for every 1 mm increase in rainfall intensity, an amount of 3.6 μg/ study location.

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location can be found from Aruna et al., 2013, 2014. A flow rate of 5 l/
m is maintained with a cyclone top fixed upside down to the inlet of the
instrument to allow the aerosols up to 2.5 microns size. It is reported by
World Meteorological Organization (WMO) that the aerosol measure-
ments need to be carried out at the relative humidity less than 40%
(WMO, 2003) and to maintain this, a diffusion drier is required to
maintain the relative humidity below 40% (Ran et al., 2016). Also, the
room temperature of the aerosol instrument should be maintained
above the dew point temperature so as to avoid the condensation of
water particles which will affect the aerosol measurements. We have
not used any drier before the aerosol sampling in the present study. The
ambient room temperature is kept around 26 °C which is above the dew
point temperature. It is also reported that the BC aerosols are hydro-
phobic in nature and not dependant on the ambient relative humidity or
the initial aerosol size (Forster et al., 2007; McMeeking et al., 2011;
Esteve et al., 2014). Arnott et al. (2003) reported that light absorption
shows uncertainties at high RH values (> ∼80%) with filter based
techniques, especially when RH changes rapidly and suggested caution
while interpreting the data in such conditions. In the present study, the
RH changes are not rapid as it varied from 70 to 95% during rainy and
non-rainy days. Further, in the present study the difference in BC
concentration between rainy and non-rainy days is found to be quite
substantial and as such it is unlikely to be accounted by RH changes. So
the main conclusions of the present study may not be affected by this
aspect. Optical attenuation technique is used to measure the BC mass
concentration and the threshold for the optical attenuation is suggested
in the range of 75–125. In the present study, we use the threshold of 75,
i.e an optical absorption value of 0.75 (Hansen, 2005). It is also re-
Fig. 3. (a & b). Mean diurnal variation of BC wavelength exponent (γ) for a)
ported that the BC measurement suffers by filter based techniques due
Oct–Dec 2015 and b) Oct–Nov 2017
to its inherent artifacts (Collaud Coen et al., 2010; Ran et al., 2016). An
error of 5% is given in the Black Carbon measurement by the manu-
facturer and this error is due to the multiple scattering and shadowing
effects (Weingartner et al., 2003). In the present study, we have used
method proposed by Virkkula et al. (2007) to correct the BC from the
shadowing effect. The main sources for the BC in the present location
are found to be from the fossil fuel burning (Aruna et al., 2013).
However, we have estimated the BC wavelength exponent for the pre-
sent study period i.e for October to December 2015 and October to
November 2017 using the same methodology used in Aruna et al.
(2013). The results of this study on the source apportioning of Black
Carbon is discussed in the Results section. The BC measurements have
been carried out in the SRM institute campus which is approximately
220 m away from the national highway (NH45). The possible transport
pathways of aerosols using the Hysplit Single Particle Lagrangian In-
tegrated Trajectory model (HYSPLIT) (www.arl.noaa.gov.ready.
hysplit4html) at 500 m above the ground level at the present study
location has been reported by Aruna et al. (2013). In the present work,
we have obtained the 3 – day cluster transport pathways using the
HYSPLT at 1500 m above the ground level for the periods October to
December 2015 and October to November 2017 and are discussed. .
The hourly rainfall, air temperature and relative humidity (RH) data
have been collected from the India Meteorological Department (IMD),
Chennai located in the Nungambakkam area which is 36.6 km radial
Fig. 4. (a & b). Mean extinction due to absorption for different RH bins for a) distance from the study location for the study period.
Oct–Dec 2015 and b) Oct–Nov 2017
The Atmospheric BLH data has been obtained from the ECMWF Re
Analysis (ERA) Interim data sets for the study location. ERA provides
2. Data and method of analysis gridded atmospheric reanalysis data globally on different space scales.
More details on ERA data sets can be found from Dee et al. (2011). The
Continuous measurements of Black Carbon (BC) Mass Concentration study makes use of 0.5° × 0.5° grid resolution data, covering the study
are being carried out at SRM IST, Chennai, as a part of Aerosol location, for this purpose. The BLH height is available for every 3 h
Radiative Forcing over India (ARFI) network of ISRO Geosphere – interval of a day at 0230, 0530, 0830, 1130, 1430, 1730, 2030 and
Biosphere Programme (GBP). Aethalometer (AE-31), supplied by the 2330 h IST and the same has been used in the study.
Magee Scientific, USA is used to measure the BC mass concentration for The Ventilation Co-efficient (VC) which is the product of BLH and
every 5 min round the clock from March 2011. The data of Black the average wind speed has also been estimated using the ERA Interim
Carbon at 880 nm from the AE-31 has been considered for the present Reanalysis data for rainy and non-rainy days to examine its effect on
analysis. The details of the Aethalometer (AE – 31) and the study BC. ERA provides wind speed data at 6 h interval, the VC was estimated

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Fig. 5. (a): Daily rainfall (mm) summed from 00 hrs to 24 hrs, from 1st October to 31st December 2015 over Chennai (b): Daily rainfall (mm) summed from 00 hrs to
24 hrs, from 1st October to 3oth November 2017 over Chennai.

for every 6 h. diurnal variability with higher values during the night and lower during
the day time. These diurnal variations are mainly connected to local
atmospheric boundary layer dynamics as reported by Aruna et al.
3. Results (2013). The night time BC for the entire study period is
4.93 ± 1.04 μg/m3 while for the day time, it is 3.32 ± 0.41 μg/m3.
3.1. Mean diurnal variation of BC, possible transport pathways of aerosols The mean BC for the total period is 4.08 ± 0.63 μg/m3. The mean BC
and BC relation with RH for other stations in peninsular India where the Northeast monsoon
(October to December) prevails is about 7.05 μg/m3 (year 2014–2017)
Mean diurnal BC mass concentration in μg/m3 over the study lo- at Thiruvananthauram (Rajeevan et al., 2018), 2.33 ± 0.82 μg/m3
cation for the study period (October to December 2015 and October to (year 2010) at Anantapur (Suresh Kumar Reddy et al., 2012) and 9.13
November 2017) is shown in Fig. 1. BC over the study location has the

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Fig. 6. Average values of a) BC (μg/m3) – hourly, b) BLH (Km) – 3 h, c) Rainfall (mm) – hourly, d) air temperature (°C) – hourly, e) Ventilation Coefficient (Km2s−1) –
6 h for rainy and non – rainy days during October 2015.

μg/m3 (year 2011) (Aruna et al., 2013). The cluster pathways for Oc- to December 2015. The sources of the aerosol over the central Indian
tober to December 2015 and October to November 2017 are shown in ocean is from the transport of dust from Arabian desert as reported by
Fig. 2(a and b) respectively. The contribution of the 3 day cluster Moorthy et al. (2001) based on the INDOEX experiments carried out
pathways are also shown by percentages in Fig. 2(a and b). These during January to April 1996, 1998 and 1999. Other than these oceanic
Hysplit back trajectories at 1500 m above the ground level infer the origins, we also found contribution from the continental during the
possible remote sources of BC aerosols arriving the study location. study period where in 17.3% and 24.5% contributions are from the
Fig. 2(a and b) depict the major contribution of about 67.3% and 49.1% northern parts of India. It is reported that during post monsoon (Oc-
is from the Bay of Bengal while the contribution from Arabian Sea show tober to December), the residue burning in the agricultural areas is
6.5% and 26.2% during the year 2015 and 2017 respectively. Findings dominant in Northern India (Vadrevu et al., 2011). The aerosols gen-
of the ICARB (Integrated Campaign of Atmospheric Aerosols, gases, and erated from these burnings travel eastward from northwest India via
Radiation Budget), during summer season of 2006 revealed the sources Indo Gangetic Plain (Vijayakumar et al., 2016). The air mass trajectory
of aerosols over Bay of Bengal and Arabian Sea are from Northern analysis over different locations in India suggested that the aerosols
Arabian Sea, middle east and African continent (Reddy et al., 2008). A sources are the combinations of natural and anthropogenic of local and
contribution of 4.3% was found from the Indian ocean during October intercontinental origin (Kulshrestha and Kumar, 2014). With a view to

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Fig. 7. Average values of a) BC (μg/m3) – hourly, b) BLH (Km) – 3 h, c) Rainfall (mm) – hourly, d) air temperature (°C) – hourly, e) Ventilation Coefficient (Km2s−1) –
6 h for rainy and non – rainy days during November 2015.

understand the local sources of BC aeroosls over the study location, we Fig. 4(a and b) show the average extinction due to absorption (mainly
have estimated the wavelength exponent (γ) for the present study attributed to BC) for different RH bins during the study period. The
period. The detailed methodology for estimating γ can be found in extinction due to absorption has been estimated by multiplying the BC
Aruna et al. (2013). Fig. 3(a and b) depict the diurnal variation of γ for absorption co-efficient and the atmospheric BLH (Aruna et al., 2014).
the study period in the year 2015 and 2017 respectively. It can be seen The Fig. 4(a and b) provides the inference that the extinction due to
from the visual inspection that γ is approximately 1 during the entire absorption did not show any dependence on RH during the years 2015
study period which infers the BC is emanating from a common source and 2017. This relation shows that BC is not having affinity with the
dominated by the fossil fuel burning. The local sources of BC from the water as it is chemically inert (Golberg, 1985). However, the hydro-
fossil fuel combustion has also been reported in other sites of India phobicity of BC will be lost with the aging and this aging depends on its
viz,a, viz at Thiruvananthapuram (8.5°N, 76.9°E) (Rajeevan et al., transformation rate (Cooke and Wilson, 1996).
2018), Agarthala (23.76°N, 91.26°E) (Guha et al., 2015), Naliya
(22.23°N, 68.89°E) in summer time (Gogoi et al., 2013) and Delhi
(28.37°N, 77.12°E) (Tiwari et al., 2015). As the present study mainly 3.2. Rainfall scenario over the study location
focuses on the BC variations during the wet removal processes, we have
verified the hydrophobic nature of BC by seeing its association with RH. Fig. 5(a and b) depicts the daily rainfall (24 h starting from 00 to
24 h IST) for the months October, November, December 2015 and

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Fig. 8. Average values of a) BC (μg/m3) – hourly, b) BLH (Km) – 3 h, c) Rainfall (mm) – hourly, d) air temperature (°C) – hourly, e) Ventilation Coefficient (Km2s−1) –
6 h for rainy and non – rainy days during December 2015.

October and November 2017 respectively over Chennai. The total afternoon and continuing in the night. A few days in November i.e.
rainfall for the months October, November and December 2015 are from 16th to 21st November 2015, the rainfall activity is well spread
141.5 mm, 962.3 mm and 426.3 mm respectively (Fig. 5(a)). The over the day which is due to frontal activity. It is documented by India
monthly rainfall during October and November 2017 are 379.mm and Meteorological Department (IMD) that the deep depression in Bay of
407 mm respectively (Fig. 5(b)). In the present study, we have con- Bengal during 8th to 10th Nov 2015, low pressure in southwest Bay of
sidered a day with rainfall amount higher than 7.5 mm as a rainy day. Bengal during 12–18 November 2015 and low pressure in southeast Bay
The days with less than 7.5 mm rainfall are considered in the present of Bengal caused the heavy rainfall occurrence over Chennai. Similarly,
work as non-rainy days. Following this criterion, during the study a continuous rain activity was seen during 30th October to 4th No-
period, we found a total number of 49 rainy days (26 in the year 2015 vember 2017 which is due to the active phase of northeast monsoon
and 23 in the year 2017 (except Dec 2017)) and rest of the days are over Chennai.
non-rainy. In December 2017, there were only 2 rainy days and hence
this month is not considered in the analysis. During the year 2016, 3.3. Relation of BC and BLH during the wet removal processes
Chennai experienced only 5 rainy days. So, the year 2016 is also not
considered for the analysis. It is observed from the hourly rainfall data Fig. 6(a–c), 7(a-c) and 8(a-c) depict the hourly variation of average
that in most of the days, the rainfall activity was seen during the late BC and BLH (3 h interval), during the rainy days and non-rainy days

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Fig. 9. Average values of a) BC (μg/m3) – hourly, b) BLH (Km) – 3 h, c) Rainfall (mm) – hourly, d) air temperature (°C) – hourly, e) Ventilation Coefficient (Km2s−1) –
6 h for rainy and non – rainy days during October 2017.

along with the monthly mean rainfall for the months October, No- BLH is nearly the same during the night time on rainy and non rainy
vember and December 2015. Also shown in Figs. 6(d), 7(d) and 8(d) are days while during the daytime it is more on non rainy days. It can be
the air temperature (ºC) and Figs. 6(e), 7(e) and 8(e) are the mean seen from Figs. 6(d), 7(d) and 8(d) that the temperature (surface) in
monthly ventilation coefficients (VC) (product of BLH and wind speed). general is higher on non rainy days compared to rainy days in the
Fig. 9(a–e) and 10(a-e) show similar plots for the months October and daytime while it is about the same in the nigh time. Higher surface
November 2017. It is found from the analysis that the monthly average temperatures can be expected to lead to greater BLH values (due to
BC during October, November and December 2015 is 5.5 μg/m3, stronger thermals) as is observed and noted above. The lower BLH
5.2 μg/m3 and 5.8 μg/m3 respectively. It can be seen from Figs. 6(a), values in the daytime during rainy days can be due to the decreased
7(a) and 8(a) that, in general, during the night time the BC is less on convective instability (Parasnis and Goyal, 1990). In the months of
rainy days compared to non rainy days. On the other hand, it is about October and November 2017, similar features to the three months in
the same on rainy days and non rainy days during the daytime. A closer 2015 as described above can be discerned (shown in Figs. 9 and 10).
examination of the figures reveals that the night time contrast extends It is known that the frequency and duration of rainfall is one of the
to morning hours, upto about 0900 h. From Figs. 6(b), 7(b) and 8(b) the controlling factors that decide the BC life cycle. The inertness of BC in

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Fig. 10. Average values of a) BC (μg/m3) – hourly, b) BLH (Km) – 3 h, c) Rainfall (mm) – hourly, d) air temperature (°C) – hourly, e) Ventilation Coefficient (Km2s−1)
– 6 h for rainy and non – rainy days during November 2017.

becoming hydrophilic indicates that the removal of BC from the at- about the same BC concentration as on non-rainy days The same is
mosphere is mainly due to physical forcing like impaction processes. indicated by the ventilation co-efficient over the study location that the
Ogren and Charlson (1983) reported that the life time of Black Carbon/ ability of dilution of BC within the atmospheric boundary layer which is
Elemental Carbon is around 40 h in rainy climate and extends upto one high during the day time and less in the night time. The difference in VC
week in clean and dry climates. It may be noted from Figs. 6(c), 7(c) is, in general, high during day time from rainy to non-rainy days and is
and 8(c) that the total rain fall on rainy days is not uniformly dis- less during the night time among the same.
tributed throughout the 24 h except perhaps in November and De- In order to further examine the wet removal of BC, we have plotted
cember 2015. the product of BLH and BC for rainy and non-rainy days as scatter plots
From the above it can be inferred that on the average, BC con- for the months October, November, December 2015 (Fig. 11(a–c)) and
centration on rainy days is about the same as on non rainy days in the for October and November 2017 (Fig. 12(a and b)). Here the BLH can
day time while it is lower in the night time. As the BLH is found to be be taken to represent the available atmospheric volume for distribution
about the same during rainy and non rainy days in the nigh time, the of BC. The scatter plots for the respective months between BC and BLH
wet removal process resulted in lower BC on rainy days in the night on rainy and non-rainy days yielded to substantial significant correla-
time. However, during daytime as the BLH is lower on rainy days tions of 0.92, 0.97, 0.41, 0.93 and 0.97 during October, November and
compared to non rainy days, the decrease of BC concentration due to December 2015 and for October and November 2017 respectively. All
wet removal appears to be compensated by the decrease in available the correlations except for December 2015 are significant at 0.01 level.
atmospheric volume (in the atmospheric boundary layer), resulting in These scatter plots reveal that there is strong relation between BLH

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Fig. 12. Scatter plots of the product of BC and BLF for rainy and non-rainy days
for a) October 2017 and b) November 2017.

Fig. 11. Scatter plots of the product of BC and BLF for rainy and non-rainy days
for a) October 2015, b) November 2015 and c) December 2015.

associated with BC during rainy and non-rainy days. It can be empha-


sized that the BC accompanied by low BLH during the rainy days has
been redistributed within the atmospheric boundary layer associated by
high BC values during non – rainy days. The slopes of the scatter plots
are around 1 except for the months November 2015 and 2017 in which
the respective slopes are 2.44 and 1.71 along with the intercepts 0.17
and 0.7. The highest slopes may represent the sensitivity of BC varia-
tions to the BLH during the rainy and non-rainy days. This may be due
to the continuous rain spells that occurred during November 2015 and
2017. The continuous rainfall events, even after cleaning the atmo-
spheric BC will impact the relation of BC and BLH products during rainy
and non-rainy days. This may be studied in detail when the isolated rain
events are considered. The overall correlation for the October and Fig. 13. Scatter plots of the product of BC and BLF for rainy and non-rainy days
November 2015 and 2017 is 0.91 (Fig. 13) which is at 0.01 level of for October and November during 2015 and 2017.
significance. From Fig. 13, it can be seen that the relation is quite good
at lower and moderate levels of BC mass concentration. As the product
of BC and BLH goes high during the non-rainy days, more scatter is

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M.A. Williams et al. Journal of Atmospheric and Solar-Terrestrial Physics 182 (2019) 165–176

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Acknowledgements Guha, A., Kumar De, B., Dhar, P., Banik, T., Chakraborty, M., Roy, R., Choudhury, A.,
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The authors are thankful to Aerosol Radiative Forcing over India aerosol black carbon in relation to long range transport over Tripura in Northeast
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thankful to Dr. B.V. Krishna Murthy, Former Director, SPL for his gui- California, USA.
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lutants: Review of wet deposition scenario in South Asia. Adv. Meteorol. https://doi.
Appendix A. Supplementary data org/10.1155/2014/596041.
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