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Atmospheric Environment 45 (2011) 1940e1945

Contents lists available at ScienceDirect

Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv

Aerosol acidity and secondary organic aerosol formation during wintertime

over urban environment in western India
R. Rengarajan*, A.K. Sudheer, M.M. Sarin
Physical Research Laboratory, Ahmedabad 380 009, India

a r t i c l e i n f o a b s t r a c t

Article history: Atmospheric mass concentration of ambient PM2.5, its chemical composition and aerosol acidity have been
Received 12 October 2010 studied during the wintertime from an urban site in a semi-arid region of western India. The concentration
Received in revised form of PM2.5 ranged from 32 to 106 mg m
3 during the 30-day sampling period; and carbonaceous species (EC,
11 January 2011
OC) and water-soluble inorganic constituents (WSIC) account for w58% and w29% of the mass, respectively.
Accepted 12 January 2011

The contribution of SO2

4 to PM2.5 is signicant (Average: 17.5%) and that of NO3 is minor (Average: w2%).
The ratio of water soluble to particulate organic carbon (WSOC/OC) varies from 0.26 to 0.52 (Average: 0.41)
Keywords:
and provides evidence for the signicant role of secondary organic aerosol (SOA) in an urban environment.
Urban aerosol
Elemental and organic carbon
Measured concentration of [H]air, used as an index of aerosol acidity, varies from 0.25 to 11 mmol m
3 and
Aerosol acidity exhibits linear increase with the secondary organic carbon (SOC). Our eld-based data provide the direct
Secondary organic aerosol evidence for enhanced SOA formation at high level of acidity, consistent with laboratory studies.
2011 Elsevier Ltd. All rights reserved.

1. Introduction
Carbonaceous aerosols, consisting of elemental carbon (EC) and
organic carbon (OC), constitute a major fraction of the ne-mode
aerosol mass (PM2.5) in an urban atmosphere and signicantly
inuence the regional air quality and climate (Gelencsr, 2004). A
substantial fraction of organic aerosols, emitted from both natural and
anthropogenic sources, is secondary in nature produced by oxidation
products of volatile organic compounds (VOC) (Seinfeld and Pankow,
2003; Volkamer et al., 2006). Estimates of secondary organic aerosol
(SOA) formation based on biogenic and anthropogenic VOC uxes,
suggest their dominance over the primary component (Kanakidou
et al., 2005). Although several of the precursors originate from
industrial and automobile emission sources, the dominant fraction
of the global SOA budget is thought to originate from biogenic VOCs
(Hallquist et al., 2009 and references therein). Recent studies suggest
that SOA contribution from anthropogenic precursors, especially from
urban environment, to the global SOA budget could be signicantly
higher than the earlier estimates (de Gouw et al., 2005; Volkamer
et al., 2006). However, large discrepancies, as much as an order of
magnitude, are associated with the estimated uxes. These incon-
sistencies arise largely due to the poor understanding of the forma-
tion mechanism of SOA from the precursors (Hallquist et al., 2009).
Several laboratory experiments have demonstrated a close-link
between formation of SOA from oxidation of VOC and particle phase
* Corresponding author. Tel.: 91 79 26314314; fax: 91 79 26301502.
E-mail address: rajan@prl.res.in (R. Rengarajan).
acidity (Jang et al., 2002; Gao et al., 2004; Surratt et al., 2007; Iinuma
et al., 2009; Surratt et al., 2010; Offenberg et al., 2009). An increase
up to several fold of SOA mass from terpenes (group of biogenic
VOCs) has been observed when acidic seed particles were used in
these chamber studies. Particle-phase reactions catalyzed by H ions
leading to the formation of high molecular weight compounds have
been proposed to explain the observed enhancement (Dommen
et al., 2006; Carlton et al., 2009). Mass spectrometry and FTIR
spectrometric analysis of organic aerosols indicate that polymeric
products are present in laboratory-generated aerosols (Hallquist
et al., 2009 and references therein), which was present in ambient
aerosol to a larger extent than what had been initially speculated
(Jang and Kamens, 2001). Gao et al. (2004) have reported that an
increase in aerosol acidity causes rapid polymerization of organic
precursors resulting in higher SOA formation. Surratt et al. (2007)
have shown that SOA yield increased with increasing acidity
due to an acid hydrolysis mechanism for organosulphate formation
of biogenic VOC oxidation products (epoxides). However, real-time
measurements based on eld studies are limited for the character-
ization and quantitative assessment of the inuence of aerosol
acidity on SOA formation from the precursors (Lewandowski et al.,
2007; Hawkins et al., 2010). Also, some of the observations present
results inconsistent with the laboratory studies, suggesting that
there is no direct evidence for the relation between aerosol acidity
and SOA formation during eld measurements (Zhang et al., 2004;
Gao et al., 2006; Peltier et al., 2007). Based on off-line eld
measurements, we present results on the chemical composition of
aerosol documenting the co-variation between secondary organic

1352-2310/$ e see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.atmosenv.2011.01.026
 Author's personal copy

R. Rengarajan et al. / Atmospheric Environment 45 (2011) 1940e1945 1941

carbon (SOC) and particle phase acidity (expressed as hydrogen ion where OCmeas is the measured OC in ambient aerosols, OCpri
concentration, [H]air) in urban environment during the wintertime. the primary OC and (OC/EC)pri the primary OC/EC ratio observed
during the sampling period. In addition, WSOC measured in this
2. Experiment study serves as a potential tracer for SOA formation (Sullivan et al.,
2004; Miyazaki et al., 2006; Salma et al., 2007; Weber et al., 2007).
PM2.5 samples (particles with aerodynamic diameter <2.5 mm)
were collected on Tissuquartz lters (Pall Life Sciences) using a high- 3. Results and discussion
volume air sampler (Tisch Inc., USA) during the wintertime (from 8th
December, 2006 to 7th January, 2007) at an urban location (Ahme- 3.1. Aerosol chemical composition: dominance
dabad, 23 020 N, 72 320 E), in a semi-arid region of western India. of anthropogenic species
Samplers were operated daily for 8e10 h during day time. Aerosol
samples were also collected in summer (MayeJune are the hottest PM2.5 mass ranged from 32 to 106 mg m
3 (Average: 56 mg m
3)
months of the year for tropical India, followed by onset of southwest during the 30-day sampling in wintertime. Average chemical
monsoon) once a week (March 21 e June 13, 2007). Relative humidity composition is summarized in Fig. 1. Water-soluble inorganic species
(RH) and ambient temperature varied between 30e60% and 16e28  C constitute 29% of PM2.5 mass whereas the contribution of organic
respectively, during sampling period in winter. The corresponding matter (OC  1.6, typical urban OM/OC ratio; Turpin and Lim, 2001)
parameters in summer varied as 35e65% and 30e42  C, respectively.
Concentrations of EC and OC were measured on EC-OC analyzer
(Sunset Laboratory) using NIOSH protocol (Birch and Cary, 1996;
Rengarajan et al., 2007). An aliquot of sample lter was also treated
with Milli-Q water for extraction of water-soluble organic carbon
(WSOC) measured on TOC analyzer (Shimadzu, TOC5000A), and for
inorganic constituents (K, Ca2, Mg2, NH 2



4 , Na , SO4 , NO3 , Cl )

measured on Ion-chromatography system (DIONEX ) (Rengarajan
et al., 2007). HCO

3 in the water extract was measured on auto-titra-
tion system using xed pH (4.3) end point method (Rastogi and Sarin,
2005). All measured parameters were corrected for procedural lter
blanks. The aerosol acidity, [H]air, was determined following the
procedures of Surratt et al. (2007) and Offenberg et al. (2009). Briey,
pH of the water extract was measured immediately after the extrac-
tion using a glass electrode (Metrohm, 6.0256.100) with a precision
of 0.05 unit. The aqueous H ion concentration (Haq-extract) is
multiplied by the total volume of water used for the extraction after
making appropriate blank corrections. The average concentration of
hydrogen ion in the aerosol samples is calculated as

  .
H air
H
aq
extract  VolH2 O Volair filtered

In this study we have used quartz lters unlike the use of teon
lters reported in earlier studies (Surratt et al., 2007; Offenberg et al.,
2009). The Haq-extract for blank lters are no more than 10
6 M and
the necessary corrections were applied for samples. The measured
inorganic ionic species are also used in the thermodynamic equi-
librium model for aerosols, ISSOROPIA-II (Fountoukis and Nenes,
2007, http://nenes.eas.gatech.edu/ISORROPIA/), for calculating the
[H]air and for comparison with the experimental data. The model
was run as reverse problem in which particle-phase composition,
ambient temperature and relative humidity are used as input.
Also, positive or negative artifact in the measurement of NH 4 ion is
not addressed in this study; hence an upper limit of 20% correction
is applied for the measured NH 4 ion concentration, considering
the over all acidic nature of the samples. Positive artifact on NO
3
measurement is likely to be minimum because of the presence of
high abundances of acidic SO2
4 and hence not attempted to account
for it. Also this is more pronounced for cellulose lters and glass
ber lters compared to quartz lter which was used for this study
(Schaap et al., 2004). SOC is estimated by the EC-tracer method
assuming minimum OC/EC as the primary ratio (Castro et al., 1999;
Rengarajan et al., 2007). Using the following equation, OCsec can be
semi-quantitatively estimated for a specic region of interest:
Fig. 1. Contribution of carbonaceous and water-soluble ionic species to PM2.5 mass
OCpri EC*OC=ECpri (1) during the winter and summer. Organic matter concentration was ascertained from
measured OC and using a conversion factor of 1.6 (Turpin and Lim, 2001; Rengarajan
et al., 2007). Insoluble dust is calculated by subtracting the measured mass of OC, EC
OCsec OCmeas
OCpri (2)
and water-soluble ionic species (WSIS) from the total PM2.5 mass.
 Author's personal copy
1942 R. Rengarajan et al. / Atmospheric Environment 45 (2011) 1940e1945
and EC are 53% and 5.4% respectively. OC varied from 11 to 39 mg m
3
(organic mass: 17e62 mg m
3) and exhibits a linear trend with EC
indicating their major contribution from anthropogenic sources
(Gelencsr, 2004). The OC/EC ratio ranges between 4.0 and 8.1


(Average: 6.2). Among inorganic constituents, SO2
4 and NO3 are the
dominant acidic species derived from anthropogenic sources (SO2

4 :
3.2e23 mg m
3; NO

3
3 : 0.7e2.1 mg m ) and are largely neutralized by
NH
4 . K varies between 0.6 and 1.7 mg m

3
(Average: 0.9 mg m
3).
The overall chemical composition of PM2.5 (Fig. 1) reveals that almost
85% of the total mass is anthropogenic in origin (carbonaceous aerosol,


SO2

4 , NO3 , NH4 and K ). The unknown fraction is calculated
by subtracting the measured mass of OC, EC and water-soluble ionic
species from the total PM2.5 mass. Ca2 measured can be considered as
an index of dust contribution (Guinot et al., 2007) which shows
signicant correlation with the unknown fraction. Hence it is assigned
as dust fraction and constitutes w12%.
During the summer, PM2.5 mass ranged between 20.0 and
51.9 mg m
3 (Average: 39.2 mg m
3). OC and EC concentrations ranged
from 4.5 to 18.9 mg m
3 (Average: 7.9 mg m
3) and 0.51e3.1 mg m
3
(Average: 0.99 mg m
3); whereas the average SO2
4 and NO
3

3
concentrations were 5.9 and 0.6 mg m , respectively. In contrast to
the winter samples, the contribution of anthropogenic constituents
to PM2.5 during summer is w57% and insoluble dust component is
w40%, indicating substantial increase in the dust contribution to the
PM2.5 mass.
3.2. SOA and water-soluble organic component
The concentration of SOC, estimated by EC-tracer method, ranged
between 2 and 12.5 mg m
3, on average it accounts for w25% of
the total OC during winter. Yuan et al. (2006) have reported that the
estimated SOC based on EC-tracer method is consistently higher
compared to Positive matrix factorization method. Also, it largely
depends on the assumed primary OC/EC ratio. We have considered
minimum ratio as primary OC/EC ratio, in which contribution from
SOC cannot be completely ruled out. Hence, SOC reported in this study
can be considered as the lower limit and temporal variability can
be compared with other parameters. Water-soluble organic matter
(WSOM WSOCmeasured  1.9, typical value for urban environment;
Fuzzi et al., 2001) ranged from 7.6 to 28 mg m
3. WSOM consists of
oxygenated organic compounds containing various functional groups
such as alcohols, carbonyls, and dicarboxylic acids and considerable
fraction of the SOC is expected to be water-soluble (Fuzzi et al., 2001;
Kiss et al., 2002; Graham et al., 2002; Hallquist et al., 2009). Experi-
mental studies investigating the water solubility of urban aerosols
have indicated that anthropogenically inuenced SOA component is
almost exclusively water soluble (Weber et al., 2007; Miyazaki et al.,
2006). SOC and WSOC exhibit a signicant linear relation (r 0.80,
p < 0.001; Fig. 2) and their similar temporal variability in winter
samples suggest major contribution of SOA to WSOC; and that
WSOC can also be considered as a proxy for the SOA. WSOC/OC ratio
varied from 0.26 to 0.52 and on an average, WSOC constitutes w41% of
the total OC during the winter period. The estimated SOC was
3.3 mg m
3 during summer and average WSOC mass concentration
was 3.8 mg m
3. A similar trend between SOC and WSOC is observed
during summer as well (Fig. 2) whereas values in summer are low
compared with those in winter. Also WSOC was highly correlated with
the derived SOC, with WSOC/SOC ratios of 1.75 and 1.27 for winter and
summer respectively. These results suggest that SOC produced during
winter and summer were different in their solubility characteristics.
3.3. Aerosol acidity and SOA
Jang et al. (2002) had suggested that the SOA formation is fav-
oured by the acidic nature of pre-existing aerosols on which the
16
winter
summer
12
r = 0.80
SOC (g m )
-3
8
4 r = 0.81
0
0 4 8 12 16
-3
WSOC (g m )
Fig. 2. Scatter plot of WSOC and SOC concentrations in PM2.5 during the winter and
the summer.
heterogeneous uptake of reactive VOCs can occur. Laboratory studies
have demonstrated that acid-catalyzed heterogeneous reactions
lead to the formation of non-volatile oligomeric compounds from
the volatile carbonyl containing species (Kroll et al., 2005). Surratt
et al. (2007) have shown from a laboratory chamber study that the
mass of SOA and measured acidity of laboratory-generated aerosol
exhibit a linear relationship, the acid catalytic reactions responsible
for such an observation is expected to be through reactive uptake
of epoxydiols of precursor VOCs (Paulot et al., 2009; Surratt et al.,


2010). In this study, SO2
4 and NO3 are the dominant components
of anthropogenic origin causing acidity of the ambient aerosols and
the measured pH of the water extract (range: 4.3e6.5; Average: 4.9)
represents an overall acidic character of the ne particulate matter
during winter. In majority of the samples, HCO
3 concentration was
not detectable.
In the summer season, a substantial increase in the fractional
contribution of alkaline dust causes signicant decrease in the acidity
(Rastogi and Sarin, 2005). The pH of the water extract varied from 4.8
to 6.8 with an average value of 5.9. The measured [H]air varied from
250 nmol m
3e11 mmol m
3 during winter. The modeled [H]air
determined from ISSOROPIA-II using the measured ionic composi-
tion of water extract of aerosol samples have been compared with the
measured [H]air (Fig. 3). Although the modeled [H]air are lower by
w2 orders of magnitude than the measured data, similarity in their
variability suggests that the two sets of data can be used as an index
of aerosol acidity. Furthermore, difference in the two sets of [H]air
concentrations is due to the fact that measured [H]air represents
the extrapolation from Haq-extract and the modeled [H]air is the
concentration derived based on measured ionic composition
assuming a thermodynamically equilibrated gas-aerosol system.
Daily variation of the modeled [H]air determined from ISSOROPIA-II
using the measured ionic species and computed SOC concentration
of the aerosol samples at Ahmedabad during the study period is
depicted in Fig. 4. The [H]air shows an increasing trend and attains
a maximum value (60 nmol m
3), and then decreases. SOC mass
concentration also increased from w4.5e13 mg m
3 during this
period, suggesting that SOC abundance increases substantially at
higher [H]air.
 Author's personal copy

R. Rengarajan et al. / Atmospheric Environment 45 (2011) 1940e1945 1943

70 18 acidity by NH 2

4 /SO4 ratios in the samples while our observation is
based on measured Haq-extract and modeled [H]air which are more

Measured [H ]aerosol (mol m )

Modeled [H+]aerosol (nmol m-3)

-3
16
60
reasonable representations of acidity. Likewise, Gao et al. (2006)
14
50 suggested that there is no evidence for oligomer formation and
12 found no correlation between particle acidity and the detected polar
40 organic species measured in the samples from southeastern United
10
States; wherein the aerosol acidity was assessed by measured NH 4,

+
30 8

SO2
4 and NO3 . Lewandowski et al. (2007) have reported higher
6
20 PM2.5 and organic aerosol mass concentration under acidic condition
4 in an urban location at North Carolina, USA where the acidity was
10
2 assessed by difference in charge balance of measured water-soluble
0 inorganic species. However, it is noteworthy that the NH 2

4 /SO4
0
equivalent ratio does not exhibit a consistent relationship with SOC
or WSOC during our observation period (Fig. 4). In previous labora-
06

06

06

06

06

06

06

06

06

06

06

06

07

07

07
tory studies by Surratt et al. (2007) and Offenberg et al. (2009),
0

0
/2

/2

/2

/2

/2

/2

/2

/2

/2

/2

/2

/2

/2

/2

/2
the measured aerosol acidity was between 100 and 1000 nM m
3
2

1
/1

/1

/1

/1

/1

/1

/1

/1

/1

/1

/1

/1

/0

/0

/0
08

10

12

14

16

18

20

22

24

26

28

30

01

03

05

which clearly demonstrated enhancement of SOA from biogenic

Fig. 3. H ion concentration, determined from the measured pH of aerosol water
VOCs. In our eld studies the [H]air observed are similar and
extract, shows signicant correlation with the modeled pH of aerosols (Fountoukis and
Nenes, 2007).
hence the precursors could be similar biogenic VOCs, considering
that agricultural and forest areas are located in the upwind region of
the sampling location. However, there is no data available from the
We thus provide direct evidence for enhanced SOA formation literature.
under favourable conditions of higher acidity derived from nss-SO2

4 , SOA is generally formed by the oxidation of VOCs which increases
indicating that acid-catalyzed condensation reactions may the polarity and hence large fraction of the resulting compounds is
contribute substantially to the formation of SOA during the winter- likely to be oxygenated making them soluble or partially soluble in
time. The modeled [H]air during summer was not found to be water (Seinfeld and Pankow, 2003; Kondo et al., 2007). This is
realistic because the water activity was insignicant as the average well reected from the increase in the WSOC concentration with
temperature was higher and the relative humidity was w50%. a parallel increase in [H]air (Fig. 4). The maximum value of the WSOC
Takahama et al. (2006) studied aerosol acidity and OC in Pittsburgh, (14.7 mg m
3) is observed on 26 December, with an increasing trend
USA for evidence of acid-catalyzed heterogeneous chemistry leading from 18 to 19 December onwards. Such comparison for the samples
to increased SOA concentrations and concluded that the effect of collected during summer is not possible because [H]air concentra-
acidity on SOA was masked by the other atmospheric processes tions both measured as well as modeled are not realistic.
occurring simultaneously. Tanner et al. (2009) examined hourly- Linear regression analysis between [H]air and SOC for the winter
collected ne particle composition data from three sites in south samples suggest a signicant correlation (r 0.82, p < 0.001; Fig. 5)
eastern United States for the evidence of SOA formation catalyzed and the linear relation can be expressed as
through aerosol acidity. Their result suggest that the acidity levels

assessed from NH 2

4 /SO4 ratios are too low to observe unequivocal SOC 0:15  H air 2:5
evidence for the same. Peltier et al. (2007) had reported that
the relationship between SOA formation and aerosol acidity is not This indicates that typically 0.15 mg of SOC is produced per nmol
meaningful during the airborne measurements conducted over coal- H. In the laboratory-based experiment by Offenberg et al. (2009),
red power plant plumes from Atlanta metropolitan region, USA. the observed SOC formation from a-pinene on photo-oxidation was
Their conclusion was based on indirect measurement of aerosol w0.015 mg per nmol H. The large difference between measure-
ments and predictions based on known precursors reveals that

1.0
2-
NH4 /SO4

0.9 +
SOC = 0.15 x [H ]air + 2.56
+

0.8
r = 0.82
0.7
10
SOC (g m )
-3

0.6

0.5
20 14
[H ]aerosol (nmol m )
-3

60 18
12
WSOC (g m )
-3

SOC (g m )
-3

16

40 14
10 5
12 8

20 10 6
+

8
4
0 6

4
2 0
2 0 0 10 20 30 40 50 60
07

07
06

06

06

06

07
06

06

06
06

06

06

06

06

+ -3
/20

/20

/20

Modeled [H ]air (nmol m )

/20

/20

/20

/20
/20

/20

/20
/20

/20

/20

/20

/20

/1 2

/0 1

/0 1

/0 1
/1 2

/1 2

/1 2

/12

/1 2
/1 2

/ 12

/1 2

/1 2

/1 2

/1 2

30

01

03

05
18
08

20

22

24

26

28
10

12

14

16

Fig. 5. Linear regression of SOC vs. modeled [H]air concentration for the winter
Fig. 4. Temporal variability in [H]air, as determined from the measured pH of water samples. Modeled [H]air concentrations for summer samples are <1 nmol m
3 and
extracts, along with WSOC and SOC concentration at an urban site (Ahmedabad). Also average SOC (represented as open circle) is 3.25 mg m
3. This is represented as open
shown is the daily variation of NH 2

4 /SO4 equivalent ratio in the ne aerosols. circle.
 Author's personal copy
1944 R. Rengarajan et al. / Atmospheric Environment 45 (2011) 1940e1945
50
40 r = 0.67
c = 11
OC (g m )
-3
30
20
10
0 compositional changes with key physical properties (e.g., volatility,
0 5 10 15
2- -3
SO4 (g m )
Fig. 6. Scatter plot of OC and SO2
4 concentrations in PM2.5 during the wintertime.
Encircled data is not considered for the regression. The non-zero intercept suggests the
occurrence of primary organic carbon.
there is a substantial amount of missing SOA especially in urban
environments (Heald et al., 2005; de Gouw et al., 2005; Volkamer
et al., 2006). Analysis of such empirical relationship between SOC
mass and [H]air in different environmental conditions is useful for
regional and global scale models to decrease the discrepancy
between the model prediction and observation of SOA. During
summer, however, a combination of aerosol composition and low
RH often induced solid-phase transitions in the aerosol (Khlystov
et al., 2005), leading to lower concentrations of acidity.
High OC measured in these samples coincided with the peak
SO2
2

4 concentration. A plot of OC and SO4 gives a positive corre-
lation (r 0.67, p < 0.001; Fig. 6). It is earlier observed that SOA
yield increased with increasing acidity due to an acid hydrolysis
mechanism for organosulphate formation of biogenic VOC oxida-
tion products (epoxides) (Surratt et al., 2007; Minerath and Elrod,
2009; Hawkins et al., 2010). It should be noted that [H]air is not
only a function of the SO2
4 concentration but also the amount of
neutralizing base (predominantly NH3 in this area), the presence
of other acidic species (e.g., NO

3 ), and also the water content of the
aerosol. A detailed evaluation of the uptake of inorganic acidic
species and precursor VOCs by ne aerosols from urban environ-
ment to form organosulphate derivatives would be crucial to
understand the inuence on the budgets of reactive VOCs, as well
as the radiative properties of the particles during the sampling
period.
4. Conclusions
Aerosol acidity, [H]air, SOC mass concentration have been
studied based on the aerosol chemical composition during winter
from an urban location (Ahmedabad) in western India. Our assess-
ment of secondary organic carbon (SOC) by the EC-tracer method
and the measured [H]air as well as that computed using an aerosol
thermodynamic equilibrium model, ISSOROPIA-II, show signicant
positive correlation suggesting that acidity favours the formation of
secondary organic aerosol (SOA) in the urban source region during
winter. During summer, this relationship is not conspicuous because
acidity is not signicantly pronounced. Water-soluble organic
carbon (WSOC) has also been used as an independent measure of
SOA. Surratt et al. (2007, 2008, 2010) proposed that aerosol acidity
arising due to high SO2
4 concentration in an urban environment
may lead to the formation of organosulphates. The role of aerosol
acidity in SOA formation has been studied in laboratory experiments,
by measuring the presence of organosulphates from natural VOCs
(Surratt et al., 2008, 2010); however, the reaction pathways and
feasibility for formation from anthropogenic VOCs in ambient
atmosphere need further investigation.
Our observation based on ambient measurements of chemical
parameters is signicantly important for quantitative assessment of
the factors controlling the chemical pathways for the SOA forma-
tion. In a rapidly growing scenario of anthropogenic activities and
emissions from mega-cities, the increase in aerosol acidity leading
to enhance formation of SOA has implications to poor air-quality
and regional changes in atmospheric chemistry. Furthermore,
formation of SOA with increase in aerosol acidity and its repre-
sentation in the regional models is essential in order to link the
20 hygroscopicity, light absorption) of the ambient aerosols in an
urban environment.
Acknowledgments
We gratefully acknowledge the ISRO-Geosphere-Biosphere Pro-
gramme ofce (Bangalore, India) for providing the nancial support.
We are grateful to two anonymous reviewers for their helpful
comments on the manuscript.
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