Aerosol Black Carbon Over A Tropical Coastal Station in India

You might also like

Download as pdf or txt
Download as pdf or txt
You are on page 1of 4

GEOPHYSICAL RESEARCH LETTERS, VOL. 29, NO. 23, 2098, doi:10.

1029/2002GL015662, 2002

Aerosol black carbon over a tropical coastal station in India


S. Suresh Babu and K. Krishna Moorthy
Space Physics Laboratory, Vikram Sarabhai Space Centre, Trivandrum, India
Received 12 June 2002; revised 27 July 2002; accepted 5 August 2002; published 5 December 2002.
[1] Extensive ground based measurements of aerosol Black tropical Indian Ocean [Lelieveld et al., 2001; Ramanathan
Carbon (BC) and size segregated aerosol mass concentration et al., 2001a; Krishnan and Ramanathan, 2002].
(total) were carried out (during August 2000 to October [3] In this paper, we present for the first time from a
2001) for the first time at a tropical coastal station, tropical coastal location in India (Trivandrum, 8.55N;
Trivandrum, India. BC depicted diurnal (with a nocturnal 77E), the results of comprehensive measurements of aero-
peak and mid-after noon low) and seasonal variations sol BC, simultaneous with total aerosol mass concentration
(highest during local winter and lowest during monsoon). obtained using a 10-channel Quartz Crystal Microbalance
The diurnal variations were closely associated with the (QCM) impactor. The temporal characteristics and its asso-
boundary-layer dynamics. Daily mean BC concentration as ciation to prevailing atmospheric processes are examined.
high as 6 mg m 3 was observed on several occasions. Mass The mass-fraction of BC, its annual variation, and their
apportionment showed a BC share ranging from 3% to as possible implications are discussed.
high as 12% to the total aerosol mass, depending on the
season. The presence of such large amount of BC over land 2. Experimental Set Up and Database
might influence the regional aerosol forcing. INDEX [4] Continuous and near-real-time measurements of the
TERMS: 0305 Atmospheric Composition and Structure: Aerosols mass concentration of aerosol BC were carried out for 15
and particles (0345, 4801); 1610 Global Change: Atmosphere months from August 2000 to October 2001, using an
(0315, 0325); 0345 Atmospheric Composition and Structure: Aethalometer; model AE-21 of Magee Scientific, USA.
Pollution—urban and regional (0305); 3322 Meteorology and The instrument aspirates ambient air from an altitude of 3
Atmospheric Dynamics: Land/atmosphere interactions. m above the ground using its inlet tube and its pump. The BC
Citation: Babu, S. S., and K. K. Moorthy, Aerosol black carbon mass concentration is estimated by measuring the change in
over a tropical coastal station in India, Geophys. Res. Lett., 29(23), the transmittance of a quartz filter tape, on to which the
2098, doi:10.1029/2002GL015662, 2002. particles impinge. Details are available elsewhere [Babu and
Moorthy, 2001; http://www.mageesci.com/Aethalometer_
1. Introduction book_2009.pdf ]. The instrument was operated at a time base
of 5 min, round the clock. The sampling location was
[2] Aerosol Black Carbon (BC), the optically absorbing Thumba, Trivandrum, situated 10 km north west of the
part of carbonaceous aerosols, is the major anthropogenic city of Trivandrum (with a population of 1 million); 500
component of atmospheric aerosol system which has sig- m east off the Arabian Sea Coast. The location is a fairly flat,
nificantly different optical and radiative properties, as com- sandy, coastal terrain with scattered vegetation. More details
pared to the other normal constituents. Due to its large are given in an earlier paper [Pillai and Moorthy, 2001].
absorption over a wide wavelength range, it could offset Being located within the rocket launch facility of Indian
significantly or even reverse the ‘‘white house’’ effect, due Space Research Organisation, there are no significant indus-
to aerosol scattering [Schwartz, 1996; Haywood and Shine, trial or domestic combustion activities for several kilometres
1997]. All the recent major field campaigns of the last around the station and hence the BC values are more
decade have ascertained the importance of BC in climate representative of the region (at least in a meso-scale).
change studies [Ramanathan et al., 2001a]. Burning of [5] Complementary data on ambient total aerosol mass
biomass and fossil fuels, automobile exhaust, aircraft emis- concentration (Mt) were obtained from near simultaneous,
sions and forest fires are the chief sources of BC. Significant but less frequent measurements, using the QCM impactor
amount of BC, if present in rain clouds, can lead to (type PC-2 of California measurements). The QCM data,
increased absorption of solar radiation, resulting in heating collected at nearly hourly intervals on 4 to 5 days a month
and eventually ‘‘burn off’’ of the clouds [Ackerman et al, with the sampling duration varying between 3 and 5 min,
2000]. Being mostly in the sub micron range, it is easily yielded total mass concentration and mass size distribution
inhaled and can be a health hazard [Horvath, 1993]. Due to (in the size range 0.05 to 25 mm) during each measurement
its environmental and climate significances, as well as [Pillai and Moorthy, 2001]. Further, data on meteorological
anthropogenic nature of its origin, characterisation of BC parameters such as wind speed, direction, temperature and
is attracting considerable interest in the recent years [Han- relative humidity were obtained from instruments (at 17 m)
sen et al., 2000]. Over the Indian landmass systematic and on a meteorological tower, located nearby. Daily rainfall was
extensive observations leading to its characterisation are also measured at the meteorological facility.
almost non-existent. The recent Indian Ocean Experiment
(INDOEX) has measured significant amounts of BC over 3. Results and Discussions
3.1. Temporal Variations – Annual Variations
Copyright 2002 by the American Geophysical Union. [6] BC, in general, exhibited well-defined diurnal as well
0094-8276/02/2002GL015662 as significant annual variations (Figure 1). Large concen-

13 - 1
13 - 2 BABU AND MOORTHY: AEROSOL BLACK CARBON OVER A TROPICAL COASTAL STATION IN INDIA

trations toccur during the months December – March of the


year. Generally, dry conditions prevail during this period,
with scanty rains (the total rainfall being 10% of the
annual), large diurnal oscillations in ambient temperature
and a prevailing continental airmass. Low BC concentrations
(<3 mg m 3) occur during the monsoon months of June to
September, when the station experiences extensive and wide-
spread rainfall totalling to 1000 mm (60% of the annual)
and is under the influence of a strong marine airmass [Pillai
and Moorthy, 2001]. During the dry months the mean BC
concentration is 5 mg m 3. During the monsoon months,
when its concentration is the lowest, average BC level is 1.5
mg m 3; which is comparable to the mean BC levels reported
for the suburban site, Uniontown, (at 340 m MSL) during
August 1990 [Allen et al., 1999] and the more recent mean
values [Chen et al., 2001] for another suburban site in
Maryland, USA but higher than that reported for a remote
island location [Bhugwant et al., 2001]. Based on INDOEX
measurements from Goa, Leon et al. [2001] reported an
average value of 3 ± 0.7 mg m 3 for the winter months.
Our winter values are higher than this. Besides the annual
variations, there is a well-defined diurnal variation with a Figure 2. The annual variations of BC (solid points with
broad nocturnal peak from 2100 to 0200 local time. It then error bars) concentration along with (a) the annual variations
reaches a low value at  0400, followed by a gradual increase of the monthly total rainfall (8), (b) the annual variations of
and a sharp peak around 0700– 0800. The BC concentration monthly mean diurnal temperature change (~).
decreases subsequently and the diurnal minimum is attained
in the late afternoon (1400 –1600 LT). The diurnal variation seasonal anthropogenic activities, the observed seasonal
is more pronounced during winter, when the diurnal ampli- changes would be more associated with the synoptic mete-
tude is more by a factor of 10 compared to the monsoon orology and long range transport. In Figure 2 the annual
months when the diurnal amplitude is typically 3. variations in the BC concentration is shown along with the
[7] Annual variation in BC is important, as it helps the annual variations of the monthly total rainfall (2(a)) and the
estimation of regional radiative impacts with increased monthly mean values of the diurnal temperature change, T,
accuracy. Some of the earlier observations [e.g., Chen et (the difference between the maximum and minimum temper-
al., 2001] did not find any significant annual variations, atures) in 2b. In both the panels, the individual points with
whereas our studies show strong annual variations with a error bars represents the daily mean values of BC and its
maximum to minimum ratio >3. As the measurement loca- standard deviation. Being a tropical and coastal station,
tion is not highly industrialised and is not subjected to extremes in temperature do not occur, the lowest temperature
does not go below 19C (in winter) and the highest temper-
ature (in summer) hardly exceeds 37C. Nevertheless max-
imum diurnal amplitude occurs during winter (December to
February) when T  15C. During this period, the rainfall
is scanty (bottom panel). Periods of highest BC concentra-
tions are associated with those of high T and low rainfall.
Similarly the periods of lowest BC occurs during monsoon
months when T is low (10C) and rainfall is consistently
high. The correlation analysis shows that monthly averaged
BC is positively correlated (coefficient +0.77) with T and
negatively (coefficient 0.74) correlated with monthly total
rainfall. Moreover, during the period from November to
March the station is generally under the influence of a
continental airmass while during May to September the
airmass changes to clean marine associated with the mon-
soon. Considering that the extent of anthropogenic activity is
not seasonal the bottom panel of Figure 2 is indicative of the
effect of washout during the monsoon months. High differ-
ential heating of the land coupled with the possible transport
from continental regions (further inland to Trivandrum)
enhance it during the dry months. Further, BC emissions
(particularly from heavy-duty diesel engines of trucks)
increase with increase in ambient air temperature [Chen et
Figure 1. Temporal variations of BC at Trivandrum. al., 2001] and this would also be important during the dry
Months 1 to 12 stand for January to December. BC values months. From modelling studies, Reddy and Venkataraman
for identical months in 2000 and 2001 are averaged. [1999] have shown that the average atmospheric residence
BABU AND MOORTHY: AEROSOL BLACK CARBON OVER A TROPICAL COASTAL STATION IN INDIA 13 - 3

leading to a faster dispersion and hence a dilution of BC near


the surface. This is strengthened by the reversal of surface
winds to sea breeze. Similar diurnal variations are reported
for BC (as well as other trace species such as CO) at
continental sites [Allen et al., 1999; Chen et al., 2001]. An
opposite pattern with a midday peak is observed at a high
altitude (2.5 km MSL) location [Bhugwant et al., 2001],
ascribed to the upward transport of BC due to elevation of the
boundary layer. It may however be noted that the BC may not
be totally lost from the atmosphere; but only is re-distributed
over a larger spatial extend by the boundary layer dynamics,
and hence has distinct impacts from radiative and health
perspectives. The daytime dilution of BC is advantageous
from the health perspective making the ambient air cleaner.
But, as BC gets transported to higher heights their radiative
forcing efficiency increases compared to the values when
they are near the surface (Haywood and Shine [1997]).
3.3. Mass Fraction of BC
[9] Even though BC contributes only a few percent to the
total aerosol mass, it can produce significant radiative
effects. Jacobson [2001] points out that magnitude of the
direct radiative forcing due to BC can exceed that due to
Figure 3. Diurnal variation of BC concentration (top methane, thereby making it an important species contribu-
panel), wind direction (middle panel) and wind speed ting to global warming. Recent INDOEX measurements
(bottom panel), averaged for a month. The vertical bars have reported 14% of BC in fine aerosol dry mass and 10%
through the points are the standard deviation of the mean. in coarse aerosol dry mass in the marine boundary layer
Dashed vertical lines in the top panel show the local sunrise [Lelieveld et al., 2001; Ramanathan et al, 2001b].
and sunset times for the 15th of the month. [10] Apportionment of BC is thus very important in
modelling aerosol radiative properties. Such estimates are
virtually non-existent for Indian locations. We used the Mt
time of BC is about 7 to 10 days during dry periods obtained using the QCM in conjunction with that of BC (Mb)
compared to 5 days or less during wet periods. Longer to estimate the BC fraction. As the QCM data were quite less
residence times lead to higher concentrations. frequent than the Aethalometer data, we used the monthly
mean values of Mb and Mt to evaluate the ratio Mb/Mt. The
3.2. Diurnal Variations month-to-month variation of this fraction is shown in
[8] Typical variation is shown in Figure 3 (top panel) for Figure 4. The share of BC to total mass is very high (> 9%)
January 2001. The monthly mean values of wind direction
and speed are shown in the bottom panels. The diurnal
variations are associated with local boundary layer dynamics
[Babu and Moorthy, 2001]. Being located near the coast, the
station is subjected to the land/sea breeze activity, partic-
ularly during continental airmass periods. As the land air is
more contaminated with BC its level increases during night-
time when land breeze prevails. Further, as the nocturnal
boundary layer is shallower than its daytime counter part by a
factor of 3 [Kunhikrishnan et al., 1993], and as the wind
speeds are lower during night, there is a rapid reduction in the
ventilation coefficient. This results in the confinement of
aerosols and a consequent increase in its concentration
during early night period. As night advances, the progressive
reduction in anthropogenic activities in the urban area result
in a reduction in BC generation, while the particles closer to
the surface are lost by sedimentation. There is a gradual build
up in BC from the morning and a sharp peak occurs between
7:00 and 9:00 LT almost an hour after the local sunrise. This
arises from the combined effects of (i) the well-known
fumigation effect in the boundary layer, which brings-in
aerosols from the nocturnal residual layer shortly after the
sunrise [Stull, 1988] and (ii) the morning build up of local
anthropogenic activities in the urban area from where the
wind is still directed. As the day advances, the increased solar Figure 4. Annual variation of BC mass fraction to total
heating leads to deeper and more turbulent boundary layer mass concentration.
13 - 4 BABU AND MOORTHY: AEROSOL BLACK CARBON OVER A TROPICAL COASTAL STATION IN INDIA

during dry months (December to March) and lowest during [14] Acknowledgments. This work was a part of the Geosphere
monsoon months (3 to 4%). The dry-month values are Biosphere Programme of the Indian Space Research Organization. We
thank the reviewers and Prof. R. Sridharan (SPL) for useful comments.
higher than that expected for an urban location. Even the
lowest values are higher than the values for continental References
average model [Hess et al., 1998], and are comparable to a
Ackerman, A. S., O. B. Toon, D. E. Stevens, A. J. Heymsfield, V. Rama-
continental polluted atmosphere. Such large share of BC can nathan, and E. J. Welton, Reduction of tropical cloudiness by soot,
have serious implications on surface and atmospheric radia- Science, 288, 1042 – 1047, 2000.
tive forcing. A mere 6% of soot contributes 11% to the aerosol Allen, G. A., J. Lawrence, and P. Koutrakis, Field validation of a semi-
continuous method for aerosol black carbon (Aethalometer) and temporal
optical depth [Satheesh et al., 1999]; a 35% reduction in total patterns of summertime hourly black carbon measurements in south-
solar radiation over the ocean surface and an increase of western PA, Atmos. Environ., 33, 817 – 823, 1999.
50% in atmospheric heating [Podgorny et al., 2000]. Over Babu, S. S., and K. K. Moorthy, Anthropogenic impact on aerosol black
land the impact would be higher [Haywood and Shine, 1997]. carbon mass concentration at a tropical coastal station: A case study,
Current Science, 81, 1208 – 1214, 2001.
[11] Here a mention of the uncertainty in the derived BC Bhugwant, C., M. Bessafi, E. Riviere, and J. Leveau, Diurnal and seasonal
mass-fraction is warranted. Extensive field studies using the variation of carbonaceous aerosols at a remote MBL site of La Reunion
Aethalometer for BC measurements and their intercompar- island, Atmos. Res., 57, 105 – 121, 2001.
Chen, L. W. A., B. G. Doddridge, R. R. Dickerson, J. C. Chow, P. K.
ison with other analytical techniques have yielded excellent Mueller, J. Quinn, and W. A. Butler, Seasonal variations in elemental
agreement [Allen et al., 1999; Im et al., 2001]. Considering carbon aerosols, carbon monoxide and sulfur dioxide: Implications for
these along with our operational configuration of the sources, Geophys. Res. Lett., 28, 1711 – 1714, 2001.
Hansen, J., M. Sato, R. Reudy, A. Lacis, and V. Oinas, Global warming in
Aethalometer, we attribute an uncertainty of 10% (with a the 21st century: An alternative scenario, Proc. Nat. Acad. Sci., 97,
minimum of 100 ng m 3) for the BC mass. This is also 9875 – 9880, 2000.
comparable to the uncertainty in the Mt estimates using the Haywood, J. M., and K. P. Shine, Multi-spectral calculations of the radia-
QCM. Combining these two the overall uncertainty in the tive forcing of tropospheric sulphate and soot aerosols using a column
model, Q. J. R. Meteorol. Soc., 123, 1907 – 1930, 1997.
BC mass-fraction would be 14%. Hess, M., P. Koepke, and I. Schult, Optical properties of aerosols and
[12] The large annual variation in BC fraction in our study clouds: The software package OPAC, Bull. Ame. Meteor. Soc., 79,
cannot be fully attributed to local anthropogenic activity, (as 831 – 844, 1998.
Horvath, H., Atmospheric light absorption – A review, Atmos. Environ.,
there are no seasonally preferred combustion activities in and 27A, 293 – 317, 1993.
around the study region). It should be a combined effect of Im, J. S., V. K. Saxena, and B. N. Wenny, An assessment of hygroscopic
synoptic meteorology (see 3.1.) and long-range transport. growth factors for aerosols in the surface boundary layer for computing
direct radiative forcing, J. Geophys. Res., 106, 20,213 – 20,224, 2001.
From Along Track Scanning Radiometer (ATSR) data, Leon Jacobson, M. Z., Strong radiative heating due to the mixing state of black
et al. [2001] reported a substantial increase in the occurrence carbon in atmospheric aerosols, Nature, 409, 695 – 697, 2001.
of forest fires over India during January – March period. Jha, B., and T. N. Krishnamurti, Real-time meteorological atlas during the
These, though occur very far away from our location, could INDOEX-1999, FSU report #99-09, Tallahassee, FL 32306-4520, USA,
1999.
still be important due to the increased atmospheric life time of Krishnan, R., and V. Ramanathan, Evidence of surface cooling from
BC in dry months, the continental nature of the airmass and absorbing aerosols, Geophys. Res. Lett., 29, 541 – 544, 2002.
the potential role of trajectories [Jha and Krishnamurti, Kunhikrishnan, P. K., K. S. Gupta, R. Ramachandran, W. J. Prakash, and
K. N. Nair, Study on thermal internal boundary layer structure over
1999]. Further, the number of vehicles in India has increased Thumba, India, Ann. Geophys., 11, 52 – 60, 1993.
from 2 million during 1970 to 38 million during 1998 Lelieveld, J., et al., The Indian Ocean Experiment: Widespread air pollution
[Satheesh, 2002]. Consequent increase in emissions would from south and south east Asia, Science, 291, 1031 – 1036, 2001.
Leon, J. F., et al., Large-scale advection of continental aerosols during
be contributors to the regional aerosol loading. INDOEX, J. Geophys. Res., 106, 28,427 – 28,439, 2001.
[13] The large amount of BC raises the following issues. Pillai, P. S., and K. K. Moorthy, Aerosol mass-size distributions at a tropical
The reduction in solar flux at the surface due to scattering coastal environment: Response to mesoscale and synoptic processes,
and absorption might reduce the sensible heat flux, and Atmos. Environ., 35, 4099 – 4112, 2001.
Podgorny, I. A., W. C. Conant, V. Ramanathan, and S. K. Satheesh, Aerosol
reduce the amount of photo synthetically active radiation modulation of atmospheric and surface solar heating rates over the Tro-
reaching the surface, which would in turn affect the crop pical Indian Ocean, Tellus, 2000.
production. The lower atmospheric heating due to BC Ramanathan, V., P. J. Crutzen, J. T. Kiehl, and D. Rosenfeld, Aerosols,
climate and the hydrological cycle, Science, 294, 2119 – 2124, 2001a.
absorption simultaneous with surface reduction in solar flux Ramanathan, V., et al., Indian Ocean Experiment: An integrated analysis of
would intensify low-level inversion, which would slow the climate forcing and effects of the great Indo-Asian haze, J. Geophys.
down convection and in turn cloud formation. These effects Res., 106, 28,371 – 28,398, 2001b.
Reddy, M. S., and C. Venkataraman, Direct radiative forcing from anthro-
are likely to influence regional aerosol radiative forcing. pogenic carbonaceous aerosols over India, Current Science, 76, 1005 –
1011, 1999.
4. Conclusions Satheesh, S. K., Aerosols and Climate, Resonance, 7, 48 – 59, April, 2002.
Satheesh, S. K., V. Ramanathan, X. L. Jones, J. M. Lobert, I. A. Podogorny,
1. Average BC concentration at Trivandrum is compar- J. M. Prospero, B. N. Holben, and N. G. Leob, A Model for the natural
able to the values reported for suburban locations. and anthropogenic aerosols for the tropical Indian ocean derived from
Indian ocean Experiment data, J. Geophys. Res., 104, 27,421 – 27,440,
2. The share of BC to the total mass concentration varies 1999.
from 10% during dry months to 3% during monsoon Schwartz, S. E., The white house effect-Short wave radiative forcing of
months. The high values though are lower than those climate by anthropogenic aerosols-An overview, J. Aerosol Sci., 27,
359 – 382, 1996.
reported during the INDOEX, are higher than the model Stull, , An introduction to boundary layer meteorology, Kluwer Academic
values for ‘continental polluted’ aerosols types. Publishers, Dordrecht, 1998.
3. BC exhibits well-defined diurnal and annual varia-
tions. Diurnal variations are mainly attributed to local
factors and boundary layer dynamics, whereas annual S. S. Babu and K. K. Moorthy, Space Physics Laboratory, Vikram
variations are more associated with airmass types. Sarabhai Space Centre, Trivandrum 695022, India. (k-k-moorthy@eth.net)

You might also like