Science of the Total Environment 744 (2020) 140359

Contents lists available at ScienceDirect

Science of the Total Environment

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

Isotope constraints of the strong influence of biomass burning to

climate-forcing Black Carbon aerosols over Southeast Asia
Junwen Liu a,b,c,f, August Andersson c, Guangcai Zhong b, Xiaofei Geng b, Ping Ding d, Sanyuan Zhu b,
Zhineng Cheng b, Mohamad Pauzi Zakaria e, Chui Wei Bong e, Jun Li b, Junyu Zheng a,f,
Gan Zhang b,⁎, Örjan Gustafsson c,⁎
a
Institute for Environmental and Climate Research, Jinan University, Guangzhou, China
b
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, China
c
Department of Environmental Science, Bolin Centre for Climate Research, Stockholm University, Stockholm, Sweden
d
State Key Laboratory of Isotope Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, China
e
Institute of Ocean and Earth Sciences, University of Malaya, Kuala Lumpur, Malaysia
f
Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Jinan University, Guangzhou, China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• We performed a one-year sampling

campaign for BC observation in a recep-
tor site of SE Asia.
• 14C measurements showed that ~50% of
BC was contributed by biomass burning
on average during the sampling period.
• The contribution of biomass burning in
BC significantly increased in the spring
season.

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

Article history: Black Carbon (BC) deteriorates air quality and contributes to climate warming, yet its regionally- and seasonally-
Received 19 April 2020 varying emission sources are poorly constrained. Here we employ natural abundance radiocarbon (14C) mea-
Received in revised form 17 June 2020 surements of BC intercepted at a northern Malaysia regional receptor site, Bachok, to quantify the relative bio-
Accepted 17 June 2020
mass vs. fossil source contributions of atmospheric BC, in a first year-round study for SE Asia (December 2015–
Available online 3 July 2020
December 2016). The annual average 14C signature suggests as large contributions from biomass burning as
Editor: Pingqing Fu from fossil fuel combustion. This is similar to findings from analogous measurements at S Asian receptors sites
(~50% biomass burning), while E Asia sites are dominated by fossil emission (~20% biomass burning). The 14C-
Keywords: based source fingerprinting of BC in the dry spring season in SE Asia signals an even more elevated biomass burn-
Black Carbon ing contribution (~70% or even higher), presumably from forest, shrub and agricultural fires. This is consistent
Radiocarbon with this period showing also elevated ratio of organic carbon to BC (up from ~5 to 30) and estimates of BC emis-
Biomass burning sions from satellite fire data. Hence, the present study emphasizes the importance of mitigating dry season veg-
SE Asia etation fires in SE Asia.
© 2020 Elsevier B.V. All rights reserved.

⁎ Corresponding authors.
E-mail addresses: zhanggan@gig.ac.cn (G. Zhang), orjan.gustafsson@aces.su.se (Ö. Gustafsson).

https://doi.org/10.1016/j.scitotenv.2020.140359
0048-9697/© 2020 Elsevier B.V. All rights reserved.
2 J. Liu et al. / Science of the Total Environment 744 (2020) 140359
1. Introduction
Black Carbon (BC) aerosol, formed from incomplete biomass and
fossil fuel combustion, is detrimental for human health (Janssen
et al., 2012) and a strong climate warming agent (Ramanathan and
Carmichael, 2008; Bond et al., 2013; Stocker et al., 2013). However,
BC emission inventories (BC-EI) give divergent estimates on the
emissions from different sources (Bond et al., 2013, Wang et al.,
2014a, 2014b, Klimont et al., 2017), largely due to its multiple emis-
sion sources and highly variable emission factors. For instance, it was
concluded that the global BC-EI differs by more than a factor of 10
(2000 Gg–29,000 Gg yr−1) with the largest uncertainty from open
burning (Bond et al., 2013). Consequently, EI-driven atmosphere-
chemistry models frequently fail to reproduce atmospheric BC con-
centrations and its seasonal pattern (Wang et al., 2011, Li et al.,
2016a, 2016b, Mues et al., 2018, Winiger et al., 2019). Moreover,
there is a systematic underestimation by factors 2–3 of the BC-
related aerosol absorption optical depth (AAOD) by general
circulation climate models (GCM) relative to estimates based on
atmospheric observations (Gustafsson and Ramanathan, 2016;
Chen et al., 2017). This implies that model estimates of direct-
radiative-forcing (DRF) for BC are likely also systematically too low
(Jacobson, 2000; Koch et al., 2007; Stocker et al., 2013; Wang et al.,
2014a, 2014b). In contrast, large-scale observation-based investigations
(Ramanathan and Carmichael, 2008) and comprehensive assessment
studies (Bond et al., 2013) conclude that the global-average BC-DRF
values are as high as 0.9 W m−2. The high uncertainty of BC-EI is
one of the most important factors influencing the uncertainty in
model-based BC-DRF (Gustafsson and Ramanathan, 2016). An accurate
quantification of the sources of ambient BC, based on observations, will
guide improved assessments of both climate and air-quality effects, yet
such studies remain poorly reported around the world, especially in
background regions.
Fig. 1. The geographic position of the sampling site (Bachok, Malaysia) and the averaged aerosol optical depth (AOD) at 550 nm obtained from the Moderate Resolution Imaging
Spectroradiometer (MODIS) satellite product from December 2015 to December 2016. The maximum AOD is set to 0.5 in this map.
SE Asia is an important source region of BC and the region often faces
severe air pollution (Vadrevu et al., 2014; Lee et al., 2016). It is well-
known that biomass-burning induced haze pollution has become a re-
curring phenomenon and draws a lot of scientific and public attention
in SE Asia. This large-scale haze is believed to mainly originate from un-
controlled wildfires yet in unknown proportions. It can extensively im-
pact the air quality of countries such as Singapore, Malaysia, Indonesia,
Cambodia, Vietnam, Myanmar, Laos, and Thailand, with a regional pop-
ulation of approximately 650 million. The estimates of the health risk
related to the biomass burning haze in SE Asia suggest that it is prob-
ably more carcinogenic than urban air (Betha et al., 2014). Further,
these fire activities may be underestimated in the frequently
employed remote-sensing-based techniques and atmospheric
chemical models (Miettinen et al., 2013; Campbell et al., 2016;
Cohen et al., 2017). Using multi-year aerosol optical properties
based on the MISR satellite and AERONET network, Cohen (2014)
found that the average fire-derived BC emissions in SE Asia are at
least 3 times higher than that from global fire emission database, im-
plying that the current quantification of biomass burning BC in SE
Asia remains poorly constrained and likely underestimated.
Radiocarbon (14C, half-life = 5730 y) is a powerful tool that can
be used to directly separate ambient BC into fractional contributions
from fossil fuel combustion and biomass burning (Masiello et al.,
2002; Reddy et al., 2002; Szidat et al., 2004; Gustafsson et al.,
2009). However, to the best of our knowledge, there is so far no 14C
measurements for BC aerosols reported for SE Asia, which limits
our capacity to quantitatively deconvolute the contributions from
biomass burning vs fossil fuel combustion. In this study, we present
14
C results of BC from a year-round sampling campaign of PM2.5
(particulate matter with a diameter of ≤2.5 μm) at Bachok, a back-
ground site in SE Asia. The overarching objective is to constrain the
seasonal variations of BC and quantifying the relative importance of
biomass burning to BC over background SE Asia.
 J. Liu et al. / Science of the Total Environment 744 (2020) 140359
2. Materials and methods
2.1. Sampling campaign
The sampling site was located at Bachok Marine Research Station
(102.4° E, 6.0° N), Institute of Ocean and Earth Sciences, University of
Malaya, Pasir Puteh, Kelantan, Malaysia (Fig. 1). Bachok has an area of
280 km2 and 130, 000 inhabitants. The climate is typically tropical
with an average temperature of 25–35 °C throughout the year. The
wind circulation system is influenced by the northeast monsoon from
December to March and southwest monsoon from June to September,
respectively (Fig. 2A). In this sampling campaign, PM2.5 samples were
collected on quartz fiber filters (QFF, Pall, 8 × 10 in.) using a high-
volume sampler (1 m3/min, XTrust Instruments, Shanghai, China)
from December 2015 to December 2016. Prior to the sampling, all filters
were baked in a muffle furnace for 6 h at 450 °C in order to minimize the
potential carbon contamination. After the sampling, all filter samples
(n = 59) and the field blanks (n = 3) were folded in half, wrapped in
the same prebaked aluminum foil, and stored in a freezer at −20 °C
until analysis.
2.2. Organic carbon and Black Carbon concentration
The quantification of organic carbon (OC) and elemental carbon (EC,
i.e., the mass-based analog of BC) concentrations was performed by a
thermal-optical transmission analyzer (Sunset Laboratory, Tigard, OR,
US) following the NIOSH 5040 protocol using well-established and
quality-assured methods (Birch and Cary, 1996; Chen et al., 2013,
Andersson et al., 2015). The average concentration of OC in the field
blanks was 0.20 ± 0.05 μg/cm2, which had been subtracted in the quan-
tifications for samples. No carbon signals were detected for the BC
Fig. 2. Variations of meteorological parameters (panel A), and the concentrations of BC and
OC/BC ratio (panel B). Samples marked with the blue stars are selected for radiocarbon
measurements (n = 21).
3
determinations of the field blanks. The relative uncertainties (1 σ,
n = 4) of OC and BC were 0.4% and 2.9%, respectively.
2.3. Black Carbon isolation and radiocarbon analysis
The CO2 emitted during the BC phase of the TOT analysis method
was diverted into a separate loop and, after several stages of online pu-
rification, cryogenically trapped as detailed in our previous studies
(Chen et al., 2013; Winiger et al., 2019). In brief, the isolated BC fraction
was trapped using a modified Sunset Laboratory instrument at the De-
partment of Environmental Science, Stockholm University. The water
and the halogen-containing gases that may exist in the samples and in-
terfere with the 14C analysis were removed by magnesium perchlorate
and silver wool. The purified CO2 was sealed in a quartz tube (L:
60 mm, OD: 6 mm, ID: 4 mm) with an inner liner inside (L: 20 mm,
OD: 3 mm, ID: 2 mm) that contained 10–11 mg Zn (Aldrich), 3–5 mg
TiH2 (Alfa Aesar), and 4–5 mg Fe catalyst (Alfa Aesar) (Chen et al.,
2013; Liu et al., 2017). The graphitization process and the 14C measure-
ments were performed at the Guangzhou Institute of Geochemistry,
Chinese Academy of Sciences using a compact accelerator mass spec-
trometry (AMS) facility (NEC, 0.5 MV) (Zhu et al., 2015).
All 14C results were given in the unit fractions of modern carbon (fM),
i.e., the fraction of the 14C/12C ratio relative to that of the reference year
of 1950 (Stuiver and Polach, 1977), and have been corrected for isotopic
fractionation. The relative uncertainty of fM values was in the range of
0.9% to 8.0%, with an average of 2.1% (n = 21, Table S1). To eliminate
the bomb tests in the 1960s, fM values need to be converted to the frac-
tion of biomass burning (fbb) as follows:
f bb ¼ f M =f M;ref
fM, ref is the reference value of fM for biomass burning activities. In
this study, fM, ref was taken as 1.11 ± 0.04 with a consideration of both
the 14C levels of atmospheric CO2 in the background site (Levin and
Kromer, 2004; Levin et al., 2013) and the relative contributions of bio-
mass with different ages. A slight difference may exist among studies
for the estimations of fM, ref values due to the unknown age of the
burned biomass in the research area (Wiggins et al., 2018), yet this un-
certainty is insignificant relative to the overall large dynamic range in
14
C between modern and fossil sources and thus have little influence
on the BC source apportionment.
3. Results and discussion
3.1. BC concentrations and OC/BC ratios in SE Asia
During December 2015 to December 2016 campaign at Bachok,
the BC concentrations varied in the range of 0.19–1.55 μgC/m3
(Fig. 2B). The 10%, 50%, and 90% percentile values for BC concentra-
tions were 0.19, 0.59, and 1.43 μgC/m3, respectively, with two out-
liers higher than 1.50 μgC/m3 . As expected, this BC concentration
level was much lower than in megacities in surrounding areas such
as Bangkok (2.4–5.6 μgC/m3 ) (Sahu et al., 2011), Singapore
(1.0–4.0 μgC/m3) (Balasubramanian et al., 2003) and Kuala Lumpur
(1.1–5.5 μgC/m3) (Salako et al., 2012). Yet, our results are compara-
ble to those performed in regional sites in S and E Asia. At the
Indian Ocean receptor site of the Maldives Climate Observatory in
Hanimaadhoo (MCOH), Budhavant et al. (2018) found that the BC
concentration was in the range of ~0.2–1.2 μgC/m3 during November
2014 to May 2015, with an average of 0.59 ± 0.28 μg/m3, which is
close to the observations in this Bachok study. Similar BC concentra-
tion level (0.7 ± 0.4 μg/m3) was found in the SE Yellow Sea receptor
of the E Asian outflow based on four-year (2008–2012) observations
at Gosan, Jeju Island, Korea (Lee et al., 2015). However, the BC con-
centration in the remote high-altitude receptor site (Nam Co station)
4 J. Liu et al. / Science of the Total Environment 744 (2020) 140359

of Tibetan Plateau, in which the atmosphere may be influenced by

the air masses transported from S and SE Asia, was only 0.09 ±
0.02 μg/m3 (Li et al., 2016a, 2016b), showing a ~7-time lower level
than the Bachok results for background SE Asia.
A distinct and systematic enhancement of the OC/BC ratio was ob-
served during the sampling campaign (Fig. 2B). The OC/BC ratio
displayed a relatively constant level (3–5) during December 2015 to
February 2016, and then gradually increased during March–May 2016
to reach very high values of 30–35 in the period of 26 April–11 May
2016. This ratio then showed a downward trend to a constant level
(8–9) from the middle of June. Typically, the OC/BC ratio is relatively
lower in cities with intensive impacts from the combustion of industry
and traffic (Cao et al., 2003; Zhang et al., 2008), and elevated in situa-
tions with biomass burning or more secondary OC (SOC) formation.
However, ambient SOC formation has never been reported to reach
the extremely high OC/BC ratio observed in this study. For example, it
was found that the SOC accounted for 44–71% of OC in the unprece-
dented 2013 winter haze pollution in China, with a corresponding
value of only 3–8 for the OC/BC ratio (Huang et al., 2014).
It is noted that the beginning of this March–May period of super-
high OC/BC is coincident with also the highest BC values of the full
year (Fig. 2B), as two consecutive samples (April 26 and May 2, 2016)
with the highest BC concentration were observed in this study. Conse-
quently, the onset of this period has the by far highest total carbon
(BC + OC) aerosol loading and the corresponding relationship between
OC and BC displayed a much stronger correlation (R2 = 0.70) than for
the full period (R2 = 0.40). This period is further coincident with the
second half of the period in SE Asia of the highest temperature and low-
est humidity (Fig. 2A). Hence, we hypothesize that these super-high
OC/BC ratios in Bachok during the spring season were to a large extent
caused by intensive biomass burning, which will be further discussed
in the following text.

3.2. The 14C-based source apportionment of BC and the biomass burning

pulse
The 14C fingerprint was used to quantify the relative contributions of
biomass burning and fossil fuel combustion to BC in SE Asia (Fig. 3). The
relative contributions of biomass burning (fbb) and fossil fuel combus-
tion (fff) to total BC on an annual average basis were 51 ± 10%
(26–67%) and 49 ± 10% (33–74%), respectively. Hence, the fractional
concentration of total BC that was derived from biomass burning BC
(BCbb) varied from 0.09 to 0.89 μgC/m3 with an average value of
0.39 ± 0.21 μgC/m3. This was on an annual average at the same level
as the fossil fuel BC (BCff), which ranged from 0.10 to 0.94 μgC/m3,
with a mean of 0.37 ± 0.22 μgC/m3.
The biomass burning in SE Asia indeed plays a key role in regulating
the regional BC aerosols in the spring season (Fig. 3). The fbb values
were 46–52% (50 ± 3%, n = 5) and 44–55% (49 ± 4%, n = 8) in
winter 2015/2016 (December 2015 and January, February 2016) and
summer/autumn 2016 (June–November), respectively, displaying a
fairly constant value of fbb in these periods. However, in the spring
season, the fbb increased to 63 ± 4% (60–67%, n = 3) and this was for
the samples with the highest OC/BC ratios (April 26, May 8 and May
25). Although studies based largely on satellite data have illustrated
that the SE Asian region produces large amounts of fire-related
aerosols due to uncontrollable burnings such as agricultural clearings
and forest fire (Streets et al., 2003; Chang and Song, 2010;
Lin et al., 2013), none of these earlier reports have quantified the
actual effect on the BC mass loadings, its isotopic signals and thus
quantitative source apportionment.
Moreover, given that BCbb is less resistant to thermal oxidation
than BCff, a large portion of BCbb (i.e., ‘soft BC’) during the intensive
biomass burning period probably was quantified as OC by the
employed thermal-optical method (Elmquist et al., 2006; Hammes
et al., 2007) Hence, while a higher fbb was documented during the
Fig. 3. Time series of the fractions of biomass burning in BC, OC/BC ratios (panel A), and the
source-divided concentrations (panel B).
spring burning period than throughout the rest of the year in this
study, it is likely that the actual corresponding fbb values and the
BCbb concentrations were even higher. The presence of a substantial
‘soft BC’ fraction (here incorrectly by the Sunset method placed in
the OC pool) during the burning period is further supported by the
simultaneously enhanced ratio of benzene polycarboxylic acids
(BPCA) to BC (G. Zhong, personal communication, 2019). Besides,
Wiggins et al. (2018) recently found that it was peat burning rather
than forest fire that played a key role in creating the smoke plumes
in SE Asia in the El Niño year of 2015 when the carbon emissions
from peat fires reached ~200 Tg (Table S2). However, the peat emis-
sion for the typical year of 2016 in this study was only 5 Tg
(Table S2), suggesting that the peat burning was insignificant also
during our sampling campaign. Overall, our data indicated that the
outburst of biomass burning during the spring season in SE Asia
would strongly lift the BC fbb from ~50% to ~70% or even higher,
and probably change the regional climate due to the difference in
the optical property of the aerosols from biomass burning and fossil
fuel (Bond et al., 2013; Cui et al., 2016).
Finally, we found that the fbb values (~25%) in December 2016 were
much lower than in other periods (Fig. 3B). This phenomenon likely re-
flects the weakened fires in SE Asia during December 2016 compared to
the same period in 2015. The satellite-based emission inventory
showed that the fire-based BC was 1.28 Gg in December 2016, which
only accounted for ~30% of that in December 2015 (Table S3). Therefore,
documentation of this abnormally low fire intensity in winter 2016
suggests increased importance of BC transported from highly-
industrialized South China for this period (Fig. S1). The winter fbb for S
 J. Liu et al. / Science of the Total Environment 744 (2020) 140359
Fig. 4. Comparison of the fractions of biomass burning (%) in BC over E Asia, S Asia, and the SE Aisa. SCCO: The South China Climate Observatory; KCOG: The Korea Climate Observatory–
Gosan; MCOH: The Maldives Climate Observatory on the island of Hanimaadhoo; SINH: The Sinhagad at a mountain–top in Western India. BACH: The Bachok atmospheric observatory,
Malaysia; BACH-BB: The Bachok atmospheric observatory during the biomass burning period. Numbers in the figure are the total BC emission fluxes for the three large regions (Klimont
et al., 2017). The fractions of biomass burning data in E Asia and S Asia are obtained from the references of Chen et al. (2013), Zhang et al. (2016), and Budhavant et al. (2015), respectively.
China have been reported in similar ranges as here intercepted at
Bashok, SE Asia, with values is also in the range of 20–30% (Chen et al.,
2013; Liu et al., 2014; Andersson et al., 2015; Zhang et al., 2015).
3.3. Comparisons of the biomass burning contribution to BC between
different Asian regions
Asia is a key emission region for BC and accounts for nearly 60% of
the global BC burden (Klimont et al., 2017). There are clear geographical
differences between the major regions of Asia concerning the
observation-based contributions from fossil vs biomass burning
(Fig. 4). In E Asia, the fbb is typically in the range of ~20–25%, highlight-
ing the strong role that fossil fuel combustion plays in China. In contrast,
fbb is ~50% in S Asia, indicating a larger role for biofuel combustion and
agricultural crop residue burning. The current study finds that the SE
Asian fbb is similarly high as S Asia, with an annual-average of ~50%.
However, uniquely among these three large regions of Asia, the SE
Asia has a period (the spring) when the fbb increase to ~70% or even
higher during the biomass burning season. The satellite-based global
fire emissions database (GFED) captures qualitatively the variation of
SE Asian fbb (Fig. S2). It indicates that most fire activities in SE Asia ap-
pear outdoors such as through burnings of forest, shrubland, and agri-
cultural waste. The slight offset in time of the GFED-BC in May 2016
relative to the corresponding fbb value is probably due to the lower
time resolution (one month) of the GFED compared to the daily Bashok
filter sampling (daily). Further, some important biomass burning
sources such as indoor biofuel cooking is challenging to monitor by sat-
ellites. Taken together, to better understand the contribution of biomass
burning to the atmospheric BC loadings over SE Asia and reconcile the
gap between the observation and model, long-term 14C observation ap-
pears to be valuable.
4. Conclusions
Biomass burning is a quantitatively important source to health- and
climate-afflicting atmospheric BC in SE Asia. Natural abundance 14C iso-
tope fingerprinting demonstrated seasonally-varying year-round con-
tributions to atmospheric BC with biomass burning contributing 51 ±
10% to the annual average, increasing to as high as ~70% or even higher
in the spring season. This annual average is similar to S Asia and about a
factor of two higher fractions from biomass burning than in E Asia. This
14
C-based quantitative apportionment of biomass burning being more
important to SE Asian spring than elsewhere in Asia is likely due to
burning of forest, shrubland, and agricultural waste. This feature was
also consistent with very high ratios of OC to BC from April to May,
which is a characteristic of biomass burning. To further evaluate and di-
agnose areas for improvement of BC emission inventories, long-term
14
C observations of atmospheric BC are warranted.
5
CRediT authorship contribution statement
Junwen Liu: Conceptualization, Methodology, Software, Investiga-
tion, Writing - original draft, Writing - review & editing, Funding acqui-
sition. August Andersson: Methodology, Software, Writing - original
draft, Writing - review & editing. Guangcai Zhong: Investigation,
Resources. Xiaofei Geng: Investigation, Resources. Ping Ding: Investi-
gation. Sanyuan Zhu: Investigation. Zhineng Cheng: Investigation.
Mohamad Pauzi Zakaria: Resources. Chui Wei Bong: Resources.
Jun Li: Resources. Junyu Zheng: Resources. Gan Zhang: Conceptual-
ization, Writing - review & editing, Supervision, Funding acquisition.
Örjan Gustafsson: Conceptualization, Writing - original draft, Writing -
review & editing, Supervision, Funding acquisition.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgments
This study was supported by the National Natural Science Founda-
tion of China (grant numbers 41430645, 41877349), the International
Partnership Program of the Chinese Academy of Sciences (Grant No.
132744KYSB20170002), the SKLOG Open Research Fund (SKLOG-
201744), the Natural Science Foundation of Guangdong Province of
China (2018A050501009), the Ministry of Higher Education, Malaysia
(HiCoE Phase II Fund, grant IOES-2014D), the Swedish Research Foun-
dation VINNOVA through grant VINNMER Marie Curie Incoming Fellow
(2016-04077) as well as the Swedish Research Council (VR) project
(# 2015-03279) and a VR Distinguished Professorship Grant to Ö.G.
(# 2017-01601). We acknowledge the use of data products or imagery
from the Land, Atmosphere Near real-time Capability for EOS (LANCE)
system operated by NASA's Earth Science Data and Information System
(ESDIS) with funding provided by NASA Headquarters.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.scitotenv.2020.140359.
References
Andersson, A., Deng, J., Du, K., Zheng, M., Yan, C., Sköld, M., Gustafsson, Ö., 2015.
Regionally-varying combustion sources of the January 2013 severe haze events
over eastern China. Environmental Science & Technology 49 (4), 2038–2043.
Balasubramanian, R., Qian, W.B., Decesari, S., Facchini, M., Fuzzi, S., 2003. Comprehensive
characterization of PM2. 5 aerosols in Singapore. Journal of Geophysical Research: At-
mospheres 108, 4523. https://doi.org/10.1029/2002JD002517.
6 J. Liu et al. / Science of the Total Environment 744 (2020) 140359
Betha, R., Behera, S.N., Balasubramanian, R., 2014. 2013 Southeast Asian smoke haze: frac-
tionation of particulate-bound elements and associated health risk. Environmental
Science & Technology 48 (8), 4327–4335.
Birch, M.E., Cary, R.A., 1996. Elemental carbon-based method for monitoring occupational
exposures to particulate diesel exhaust. Aerosol Sci. Technol. 25 (3), 221–241.
Bond, T.C., Doherty, S.J., Fahey, D.W., Forster, P.M., Berntsen, T., DeAngelo, B.J., Flanner,
M.G., Ghan, S., Kärcher, B., Koch, D., Kinne, S., Kondo, Y., Quinn, P.K., Sarofim, M.C.,
Schultz, M.G., Schulz, M., Venkataraman, C., Zhang, H., Zhang, S., Bellouin, N.,
Guttikunda, S.K., Hopke, P.K., Jocobson, M.Z., Kaise, J.W., Klimont, Z., Lohmann, U.,
Schwarz, J.P., Shindell, D., Storelvmo, T., Warren, S.G., Zender, C.S., 2013. Bounding
the role of black carbon in the climate system: a scientific assessment. Journal of Geo-
physical Research: Atmospheres 118 (11), 5380–5552. https://doi.org/10.1002/
jgrd.50171.
Budhavant, K., Andersson, A., Bosch, C., Kruså, M., Kirillova, E.N., Sheesley, R.J., Safai, P.D.,
Rao, P.S.P., Gustafsson, Ö., 2015. Radiocarbon-based source apportionment of elemen-
tal carbon aerosols at two South Asian receptor observatories over a full annual cycle.
Environ. Res. Lett. 10 (6), 064004.
Budhavant, K., Bikkina, S., Andersson, A., Asmi, E., Backman, J., Kesti, J., Zahid, H., Satheesh,
S., Gustafsson, Ö., 2018. Anthropogenic fine aerosols dominate the wintertime regime
over the northern Indian Ocean. Tellus Ser. B Chem. Phys. Meteorol. 70 (1), 1–15.
Campbell, J.R., Ge, C., Wang, J., Welton, E.J., Bucholtz, A., Hyer, E.J., Reid, E.A., Chew, B.N.,
Liew, S.-C., Salinas, S.V., Lolli, S., Kaku, K.C., Lynch, P., Mahmud, M., Mohamad, M.,
Holben, B.N., 2016. Applying advanced ground-based remote sensing in the South-
east Asian maritime continent to characterize regional proficiencies in smoke trans-
port modeling. J. Appl. Meteorol. Climatol. 55 (1), 3–22.
Cao, J., Lee, S., Ho, K., Zhang, X., Zou, S., Fung, K., Chow, J.C., Watson, J.G., 2003. Character-
istics of carbonaceous aerosol in Pearl River Delta Region, China during 2001 winter
period. Atmos. Environ. 37 (11), 1451–1460.
Chang, D., Song, Y., 2010. Estimates of biomass burning emissions in tropical Asia based
on satellite-derived data. Atmos. Chem. Phys. 10 (5), 2335–2351.
Chen, B., Andersson, A., Lee, M., Kirillova, E.N., Xiao, Q., Kruså, M., Shi, M., Hu, K., Lu, Z.,
Streets, D.G., Du, K., Gustafsson, Ö., 2013. Source forensics of black carbon aerosols
from China. Environmental Science & Technology 47 (16), 9102–9108.
Chen, B., Zhu, Z., Wang, X., Andersson, A., Chen, J., Zhang, Q., Gustafsson, Ö., 2017. Recon-
ciling modeling with observations of radiative absorption of black carbon aerosols.
Journal of Geophysical Research: Atmospheres 122 (11), 5932–5942.
Cohen, J.B., 2014. Quantifying the occurrence and magnitude of the Southeast Asian fire
climatology. Environ. Res. Lett. 9 (11), 114018.
Cohen, J.B., Lecoeur, E., Ng, D.H.L., 2017. Decadal-scale relationship between measure-
ments of aerosols, land-use change, and fire over Southeast Asia. Atmos. Chem.
Phys. 17 (1), 721–743.
Cui, X., Wang, X., Yang, L., Chen, B., Chen, J., Andersson, A., Gustafsson, Ö., 2016. Radiative
absorption enhancement from coatings on black carbon aerosols. Sci. Total Environ.
551–552, 51–56.
Elmquist, M., Cornelissen, G., Kukulska, Z., Gustafsson, Ö., 2006. Distinct oxidative stabili-
ties of char versus soot black carbon: implications for quantification and environmen-
tal recalcitrance. Glob. Biogeochem. Cycles 20 (2), GB2009. https://doi.org/10.1029/
2005GB002629.
Gustafsson, Ö., Ramanathan, V., 2016. Convergence on climate warming by black carbon
aerosols. Proc. Natl. Acad. Sci. U. S. A. 113 (16), 4243–4245.
Gustafsson, Ö., Kruså, M., Zencak, Z., Sheesley, R.J., Granat, L., Engström, E., Praveen, P.S.,
Rao, P.S.P., Leck, C., Rodhe, H., 2009. Brown clouds over South Asia: biomass or fossil
fuel combustion? Science 323 (5913), 495–498.
Hammes, K., Schmidt, M.W., Smernik, R.J., Currie, L.A., Ball, W.P., Nguyen, T.H.,
Louchouarn, P., Houel, S., Gustafsson, Ö., Elmquist, M., Cornelissen, G., Skjemstad,
J.O., Masiello, C.A., Song, J., Peng, P., Mitra, S., Dunn, J.C., Hatcher, P.G., Hockaday,
W.C., Smith, D.M., Hartkopf-Fröder, C., Böhmer, A., Lüer, B., Huebert, B.J., Amelung,
W., Brodowski, S., Huang, L., Zhang, W., Gschwend, P.M., Flores-Cervantes, D.X.,
Largeau, C., Rouzaud, J.-N., Rumpel, C., Guggenberger, G., Kaiser, K., Rodionov, A.,
Gonzalez-Vila, F.J., Gonzalez-Perez, J.A., de la Rosa, J.M., Manning, D.A.C., López-
Capél, E., Ding, L., 2007. Comparison of quantification methods to measure fire-
derived (black/elemental) carbon in soils and sediments using reference materials
from soil, water, sediment and the atmosphere. Glob. Biogeochem. Cycles 21 (3),
GB3016. https://doi.org/10.1029/2006GB002914.
Huang, R.-J., Zhang, Y., Bozzetti, C., Ho, K.-F., Cao, J.-J., Han, Y., Daellenbach, K.R., Slowik,
J.G., Platt, S.M., Canonaco, F., Zotter, P., Wolf, R., Pieber, S.M., Bruns, E.A., Crippa, M.,
Ciarelli, G., Piazzalunga, A., Schwikowski, M., Abbaszade, G., Schnelle-Kreis, J.,
Zimmermann, R., An, Z., Szidat, S., Baltensperger, U., El Haddad, I., Prévôt, A.S.H.,
2014. High secondary aerosol contribution to particulate pollution during haze
events in China. Nature 514 (7521), 218–222.
Jacobson, M.Z., 2000. A physically-based treatment of elemental carbon optics: implica-
tions for global direct forcing of aerosols. Geophys. Res. Lett. 27 (2), 217–220.
Janssen, N.A., Gerlofs-Nijland, M.E., Lanki, T., Salonen, R.O., Cassee, F., Hoek, G., Fischer, P.,
Brunekreef, B., Krzyzanowski, M., 2012. Health Effects of Black Carbon, World Health
Organization Regional Office for Europe.
Klimont, Z., Kupiainen, K., Heyes, C., Purohit, P., Cofala, J., Rafaj, P., Borken-Kleefeld, J.,
Schöpp, W., 2017. Global anthropogenic emissions of particulate matter including
black carbon. Atmos. Chem. Phys. 17 (14), 8681–8723.
Koch, D., Bond, T.C., Streets, D., Unger, N., Van der Werf, G.R., 2007. Global impacts of aero-
sols from particular source regions and sectors. Journal of Geophysical Research: At-
mospheres 112, D02205. https://doi.org/10.1029/2005JD007024.
Lee, K., Kim, Y.J., Kang, C.-H., Kim, J.-S., Chang, L.-S., Park, K., 2015. Chemical characteristics
of long-range-transported fine particulate matter at Gosan, Jeju Island, in the spring
and fall of 2008, 2009, 2011, and 2012. J. Air Waste Manage. Assoc. 65 (4), 445–454.
Lee, J.S.H., Jaafar, Z., Tan, A.K.J., Carrasco, L.R., Ewing, J.J., Bickford, D.P., Webb, E.L., Koh, L.P.,
2016. Toward clearer skies: challenges in regulating transboundary haze in Southeast
Asia. Environ. Sci. Pol. 55, 87–95.
Levin, I., Kromer, B., 2004. The tropospheric 14CO2 level in mid-latitudes of the Northern
Hemisphere (1959–2003). Radiocarbon 46 (3), 1261–1272.
Levin, I., Kromer, B., Hammer, S., 2013. Atmospheric Δ14CO2 trend in Western European
background air from 2000 to 2012. Tellus Ser. B Chem. Phys. Meteorol. 65 (1).
https://doi.org/10.3402/tellusb.v65i0.20092.
Li, C., Bosch, C., Kang, S., Andersson, A., Chen, P., Zhang, Q., Cong, Z., Chen, B., Qin, D.,
Gustafsson, Ö., 2016a. Sources of black carbon to the Himalayan–Tibetan Plateau gla-
ciers. Nat. Commun. 7, 12574.
Li, K., Liao, H., Mao, Y., Ridley, D.A., 2016b. Source sector and region contributions to con-
centration and direct radiative forcing of black carbon in China. Atmos. Environ. 124,
351–366.
Lin, N.-H., Tsay, S.-C., Maring, H.B., Yen, M.-C., Sheu, G.-R., Wang, S.-H., Chi, K.H., Chuang,
M.-T., Ou-Yang, C.-F., Fu, J.S., Reid, J.S., Lee, C.-T., Wang, L.-C., Wang, J.-L., Hsu, C.N.,
Sayer, A.M., Holben, B.N., Chu, Y.-C., Nguyen, X.A., Sopajaree, K., Chen, S.-J., Cheng,
M.-T., Tsuang, B.-J., Tsai, C.-J., Peng, C.-M., Schnell, R.C., Conway, T., Chang, C.-T., Lin,
K.-S., Tsai, Y.I., Lee, W.-J., Chang, S.-C., Liu, J.-J., Chiang, W.-L., Huang, S.-J., Lin, T.-H.,
Liu, G.-R., 2013. An overview of regional experiments on biomass burning aerosols
and related pollutants in Southeast Asia: from BASE-ASIA and the Dongsha Experi-
ment to 7-SEAS. Atmos. Environ. 78, 1–19.
Liu, J., Li, J., Zhang, Y., Liu, D., Ding, P., Shen, C., Shen, K., He, Q., Ding, X., Wang, X., Chen, D.,
Szidat, S., Zhang, G., 2014. Source apportionment using radiocarbon and organic
tracers for PM2.5 carbonaceous aerosols in Guangzhou, South China: contrasting
local-and regional-scale haze events. Environmental Science & Technology 48 (20),
12002–12011.
Liu, J., Li, J., Ding, P., Zhang, Y., Liu, D., Shen, C., Zhang, G., 2017. Optimizing isolation pro-
tocol of organic carbon and elemental carbon for 14C analysis using fine particulate
samples. Atmos. Environ. 154, 9–19.
Masiello, C.A., Druffel, E.R.M., Currie, L.A., 2002. Radiocarbon measurements of black car-
bon in aerosols and ocean sediments. Geochim. Cosmochim. Acta 66 (6), 1025–1036.
Miettinen, J., Hyer, E., Chia, A.S., Kwoh, L.K., Liew, S.C., 2013. Detection of vegetation fires
and burnt areas by remote sensing in insular Southeast Asian conditions: current sta-
tus of knowledge and future challenges. Int. J. Remote Sens. 34 (12), 4344–4366.
Mues, A., Lauer, A., Lupascu, A., Rupakheti, M., Kuik, F., Lawrence, M.G., 2018. WRF and
WRF-Chem v3.5.1 simulations of meteorology and black carbon concentrations in
the Kathmandu Valley. Geosci. Model Dev. 11 (6), 2067–2091.
Ramanathan, V., Carmichael, G., 2008. Global and regional climate changes due to black
carbon. Nat. Geosci. 1 (4), 221–227.
Reddy, C.M., Pearson, A., Xu, L., McNichol, A.P., Benner, B.A., Wise, S.A., Klouda, G.A., Currie,
L.A., Eglinton, T.I., 2002. Radiocarbon as a tool to apportion the sources of polycyclic
aromatic hydrocarbons and black carbon in environmental samples. Environ. Sci.
Technol. 36 (8), 1774–1782.
Sahu, L., Kondo, Y., Miyazaki, Y., Pongkiatkul, P., Kim Oanh, N., 2011. Seasonal and diurnal
variations of black carbon and organic carbon aerosols in Bangkok. Journal of
Geophysical Research: Atmospheres 116, D15302. https://doi.org/10.1029/
2010JD015563.
Salako, G.O., Hopke, P.K., Cohen, D.D., Begum, B.A., Biswas, S.K., Pandit, G.G., Chung, Y.-S.,
Rahman, S.A., Hamzah, M.S., Davy, P., Markwitz, A., Shagjjamba, D., Lodoysamba, S.,
Wimolwattanapun, W., Bunprapob, S., 2012. Exploring the variation between EC
and BC in a variety of locations. Aerosol Air Qual. Res. 12 (1), 1–7.
Stocker, T.F., Qin, D., Plattner, G.-K., Tignor, M., Allen, S.K., Boschung, J., Nauels, A., Xia, Y.,
Bex, V., Midgley, P.M., 2013. IPCC, 2013: Climate Change 2013: The Physical Science
Basis. Contribution of Working Group I to the Fifth Assessment Report of the Inter-
governmental Panel on Climate Change. Cambridge University Press, Cambridge,
United Kingdom and New York, NY, USA (1535 pp.).
Streets, D., Yarber, K., Woo, J.H., Carmichael, G., 2003. Biomass burning in Asia: annual and
seasonal estimates and atmospheric emissions. Glob. Biogeochem. Cycles 17 (4),
1099. https://doi.org/10.1029/2003GB002040, 4.
Stuiver, M., Polach, H.A., 1977. Discussion reporting of 14C data. Radiocarbon 19 (3),
355–363.
Szidat, S., Jenk, T.M., Gäggeler, H.W., Synal, H.A., Hajdas, I., Bonani, G., Saurer, M., 2004.
THEODORE, a two-step heating system for the EC/OC determination of radiocarbon
(14C) in the environment. Nucl. Instrum. Methods Phys. Res., Sect. B 223-224,
829–836.
Vadrevu, K.P., Lasko, K., Giglio, L., Justice, C., 2014. Analysis of Southeast Asian pollution
episode during June 2013 using satellite remote sensing datasets. Environ. Pollut.
195, 245–256.
Wang, Q., Jacob, D.J., Fisher, J.A., Mao, J., Leibensperger, E., Carouge, C., Sager, P.L., Kondo,
Y., Jimenez, J., Cubison, M., Cubison, M.J., Doherty, S.J., 2011. Sources of carbonaceous
aerosols and deposited black carbon in the Arctic in winter-spring: implications for
radiative forcing. Atmos. Chem. Phys. 11 (23), 12453–12473.
Wang, Q., Jacob, D.J., Spackman, J.R., Perring, A.E., Schwarz, J.P., Moteki, N., Marais, E.A., Ge,
C., Wang, J., Barrett, S.R.H., 2014a. Global budget and radiative forcing of black carbon
aerosol: constraints from pole-to-pole (HIPPO) observations across the Pacific.
J. Geophys. Res. Atmos. 119, 195–206. https://doi.org/10.1002/2013JD020824.
Wang, R., Tao, S., Balkanski, Y., Ciais, P., Boucher, O., Liu, J., Piao, S., Shen, H., Vuolo, M.R.,
Valari, M., Chen, H., Chen, Y., Cozic, A., Huang, Y., Li, B., Li, W., Shen, G., Wang, B.,
Zhang, Y., 2014b. Exposure to ambient black carbon derived from a unique inventory
and high-resolution model. Proc. Natl. Acad. Sci. U. S. A. 111 (7), 2459–2463.
Wiggins, E.B., Czimczik, C.I., Santos, G.M., Chen, Y., Xu, X., Holden, S.R., Randerson, J.T.,
Harvey, C.F., Kai, F.M., Yu, L.E., 2018. Smoke radiocarbon measurements from
Indonesian fires provide evidence for burning of millennia-aged peat. Proc. Natl.
Acad. Sci. U. S. A. 115 (49), 12419–12424.
 J. Liu et al. / Science of the Total Environment 744 (2020) 140359
Winiger, P., Barrett, T., Sheesley, R., Huang, L., Sharma, S., Barrie, L.A., Yttri, K.E.,
Evangeliou, N., Eckhardt, S., Stohl, A., Klimont, Z., Heyes, C., Semiletov, I.P., Dudarev,
O.V., Charkin, A., Shakhove, N., Holmsrand, H., Andersson, A., Gustafsson, Ö., 2019.
Source apportionment of circum-Arctic atmospheric black carbon from isotopes
and modeling. Sci. Adv. 5 (2), eaau8052. https://doi.org/10.1126/sciadv.aau8052.
Zhang, X., Wang, Y., Zhang, X., Guo, W., Gong, S., 2008. Carbonaceous aerosol composition
over various regions of China during 2006. Journal of Geophysical Research: Atmo-
spheres 113, D14111. https://doi.org/10.1029/2007JD009525.
Zhang, Y.-L., Huang, R.-J., El Haddad, I., Ho, K.-F., Cao, J.-J., Han, Y., Zotter, P., Bozzetti, C.,
Daellenbach, K., Canonaco, F., Slowik, J.G., Salazar, G., Schwikowski, M., Schnelle-
Kreis, J., Abbaszade, G., Zimmermann, R., Baltensperger, U., Prévôt, A.S.H., Szidat, S.,
7
2015. Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities
during the extreme winter haze episode of 2013. Atmos. Chem. Phys. 15 (3),
1299–1312.
Zhang, Y.-L., Kawamura, K., Agrios, K., Lee, M., Salazar, G., Szidat, S., 2016. Fossil and non-
fossil sources of organic and elemental carbon aerosols in the outflow from Northeast
China. Environmental Science & Technology 50 (12), 6284–6292.
Zhu, S., Ding, P., Wang, N., Shen, C., Jia, G., Zhang, G., 2015. The compact AMS facility at
Guangzhou Institute of Geochemistry, Chinese Academy of Sciences. Nucl. Instrum.
Methods Phys. Res., Sect. B 361, 72–75.