Current Pollution Reports (2020) 6:440–451

https://doi.org/10.1007/s40726-020-00162-4

AIR POLLUTION (H ZHANG AND Y SUN, SECTION EDITORS)

Aerosol Measurements by Soot Particle Aerosol Mass

Spectrometer: a Review
Yunjiang Zhang 1 & Junfeng Wang 1 & Shijie Cui 1 & Dan Dan Huang 2 & Xinlei Ge 1

Published online: 18 September 2020

# Springer Nature Switzerland AG 2020

Abstract
Atmospheric aerosol particles, being composed of various types of chemical mixtures, affect significantly on human health and
climate. During the last decade, many studies were focused on characterization of chemical and physical properties as well as
source apportionment of atmospheric aerosols, which have made substantial implications for aerosol-induced air pollution and
climate mitigation. Instrumental measurement techniques provide one of the most direct and effective ways to determine aerosol
physicochemical characterization and thereby to constrain aerosol modeling. The Aerodyne soot particle aerosol mass spectrom-
eter (SP-AMS), a state-of-the-art instrument, combines the advantages of both high-resolution time-of-flight AMS (HR-ToF-
AMS) and single particle soot photometer (SP2). It can measure high-resolution chemical composition, size distribution, and
mixing state of both non-refractory and refractory aerosol particles. Specially, chemical-resolved coating materials of refractory
black carbon-containing particles can be quantified by SP-AMS. Moreover, same as HR-ToF-AMS, highly time-resolved
organic mass spectral data can be applied for further identification and quantification of organic aerosol sources with receptor
models, such as positive matrix factorization (PMF). This review summarizes results and findings obtained by recent SP-AMS
measurements in field observations and laboratory studies. These SP-AMS measurements mainly cover the topics of soot cluster
ions, trace metals, chemical composition and sources of non-refractory bulk aerosols, mixing state, and light absorption prop-
erties of black carbon-containing particles. Finally, we propose some potential prospects for future studies by using the SP-AMS.

Keywords SP-AMS . Black carbon . Trace metals . Sources . Mixing state . Radiative absorption

Introduction aerosol mixtures, black carbon-containing particles are a

Atmospheric aerosols have strong impacts on global and re-
gional air quality [1, 2] and climate change [3–5]. These im-
pacts can pose serious threat to human health [6, 7] and the
earth’s ecosystems [3]. In ambient air, fine aerosols (PM2.5)
often exist as complex mixtures, e.g., different types of aero-
sols mixed with each other to some extent. Among these
This article is part of the Topical Collection on Air Pollution
* Xinlei Ge
caxinra@163.com
1
Jiangsu Key Laboratory of Atmospheric Environment Monitoring
and Pollution Control, Collaborative Innovation Center of
Atmospheric Environment and Equipment Technology, School of
Environmental Science and Engineering, Nanjing University of
Information Science and Technology, Nanjing, China
2
State Environmental Protection Key Laboratory of Formation and
Prevention of the Urban Air Pollution Complex, Shanghai Academy
of Environmental Sciences, Shanghai, China
unique component, since black carbon itself has a net strong
warming effect [5, 8, 9] and it thereby indirectly affects air
quality via aerosol–boundary layer interactions [10, 11].
Moreover, black carbon-containing aerosols can also serve
as cloud condensation nuclei (CCN) and/or ice nuclei (IN)
[12], and thereby have significant effects on cloud formation
and lifetime as well as precipitation [9]. The growing impor-
tance of black carbon-containing particles in the atmosphere
has been witnessed by a large increase in this subject study.
During the last decades, some new instruments with state-
of-the-art analytical techniques have been developed to mea-
sure aerosol chemical and physical properties [13–15]. For
example, the aerodyne aerosol mass spectrometer (AMS)
has been widely applied to globally investigate chemical and
physical characterization of ambient non-refractory aerosol
particles [16, 17]. As reviewed by Zhou et al. (2020) [18],
there have been numerous AMS studies performed in Asia,
one of the highest anthropogenic emission regions in the
world, to characterize aerosol chemistry, physics, sources,

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Curr Pollution Rep (2020) 6:440–451
and chemical evaluation, etc. In particular, the aerodyne soot
particle AMS (SP-AMS) [19, 20]—a combined version of the
recently developed aerodyne high resolution time-of-flight
AMS (HR-ToF-AMS) [21] and single particle soot photome-
ter (SP2) [22]—was developed for direct measurements of the
chemical and physical properties of particles containing re-
fractory black carbon (rBC). In practice, the SP-AMS mea-
surements can be performed by online [23–29] or offline
[30–32] methods. Based on SP-AMS measurements, most
previous studies focused on investigation of chemical compo-
sition, sources, formation mechanisms, optical properties, and
hygroscopicity of rBC-containing particles. Thus, it can be
confirmed that this novel SP-AMS technique has been helping
the atmospheric science community to better understand
chemical and physical properties of rBC-containing particles
in ambient air. This review presents a recent account of atmo-
spheric aerosol studies based on SP-AMS measurements, as
well as some perspectives that could be further achieved using
such instrumental techniques in future.
SP-AMS Description
There are several versions of aerodyne aerosol mass spectrom-
eters (AMS), such as quadrupole AMS (Q-AMS) [33], com-
pact time-of-flight AMS (C-ToF-AMS) [34], high-resolution
time-of-flight AMS (HR-ToF-AMS) [21], and the SP-AMS
[19]. Among these versions, the SP-AMS is the most ad-
vanced and unique instrument, because it can detect both
non-refractory (including organics, sulfate, nitrate, ammoni-
um, and chloride) and refractory (e.g., soot and trace metals)
chemical components, respectively. The detailed principle of
the SP-AMS has been systematically described by Onasch
et al. (2012) [19]. Briefly, the development and design of the
SP-AMS is based on the HR-ToF-AMS. Differently, the SP-
AMS is equipped with two vaporization schemes, i.e., a stan-
dard tungsten vaporizer and an additional laser vaporizer, re-
spectively, which allows three detection modes (see Fig. 1).
One mode is for measuring the bulk non-refractory aerosols
(NR-PMbulk), which is the same as the HR-ToF-AMS. In this
measurement mode, non-refractory chemical species are de-
tected by flash vaporization of sampled particles on a heated
tungsten surface with typical temperature at around 600 °C.
The other mode includes the two vaporizers working together
(i.e., tungsten-on + laser-on), which can measure aerosol mix-
tures of both NR-PMbulk and refractory aerosol species (e.g.,
rBC and metal ions). The last mode is operated with the laser
vaporizer only, i.e., the diode-pumped Nd/YAG intracavity
laser at the wavelength of 1064 nm, which is a same laser
used in the SP2 instrument [22]. In practice, the tungsten va-
porizer has to be removed from instrument when using the
laser-only vaporizer mode. This is due to the fact that tungsten
vaporizer can still be heated, e.g., at around 200 °C, by the
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441
instrument system (e.g., filament component), which can then
yield some noise for the laser-only vaporizer detection mode.
Both non-refractory and refractory aerosol components can be
vaporized at heating temperature at around 4000 K with the
laser vaporizer. It should be noted that the SP-AMS laser-only
vaporizer mode is only for detecting particles that contain
laser light-absorbing compounds at the 1064 nm (e.g., rBC),
since only rBC-containing particles are selectively vaporized
by the laser vaporizer. In addition, trace metal ions can be
detected by the laser vaporizer mode, but these species have
also to be coated with rBC particles. The vaporized particles
via the both types of vaporizers, i.e., being generated to gas-
phase molecules, are ionized using 70 eV electron impact and
then analyzed by ToF mass spectrometer system. The ioniza-
tion and analyzing schemes of SP-AMS are the same as the
HR-ToF-AMS. The SP-AMS can also provide size distribu-
tion information of aerosol chemical compounds, which are
also the same as the standard AMS instruments [33]. By using
receptor model analysis, such as positive matrix factorization
(PMF) [35], the mass spectral data of SP-AMS non-refractory
and refractory aerosol composition can be further analyzed to
identify and quantify different source factors of these aerosols.
A particle-sizing chamber system equipped with particle time-
of-flight (PToF) chopper motor is used in SP-AMS to deter-
mine the vacuum aerodynamic diameter of aerosols particles.
Figure 2 summarizes various locations with online or offline
SP-AMS measurements for ambient samples by setting differ-
ent vaporizer detection modes.
Measurements of Refractory Carbon Ions
The SP-AMS was firstly conducted in an urban environment
in Chestnut Hill, MA, in March 2008 for ambient BC-
containing particle measurements to evaluate the instrument
performance [19]. A good agreement for measuring ambient
black carbon mass between SP-AMS and multi-angle absorp-
tion photometer (MAAP) instruments was observed, indicat-
ing a good performance of SP-AMS to quantify rBC concen-
tration [19]. Meanwhile, they also observed that the small
carbon cluster ions (C1+-C5+) dominated the rBC ion distribu-
tion, which is, however, different from laboratory-generated
soot samples that present significant fraction of larger carbon
ions (greater than C6+). In fact, such rBC ion distribution
dominated by small carbon cluster ions (C1+-C5+) for ambient
samples has been frequently reported by recent SP-AMS field
observations at various sampling sites [24, 28, 36–40]. The
different rBC ion distribution between ambient-related obser-
vation and laboratory-generated samples may reveal different
formation mechanisms of soot particle from different sources
[19, 36, 41]. Onasch et al. (2015) [36] investigated differences
in the carbon cluster (Cn+) mass spectra of 12 types of rBC-
containing particle samples (such as biomass burning, diesel
442 Curr Pollution Rep (2020) 6:440–451

SP-AMS three vaporizer modes

Tungsten Tungsten + laser Laser

NR-PMbulk NR-PMbulk, rBC, rBC, NR-PMBC, R-PMBC

NR-PMBC, R-PMBC

NR-PMbulk = non-refractory parculate material (e.g., organics, sulfate, nitrate, ammonium, and chloride)
NR-PMBC= non-refractory parculate material (same as above) coated with BC-containing parcles
rBC = refractory black carbon (including carbon cluster ions)
R-PMBC = refractory parculate material (e.g., trace metals) coated with BC-containing parcles

Fig. 1 Chemical composition measured by SP-AMS with different vaporizer modes, including tungsten, tungsten + laser, and laser, respectively

exhaust, fullerene-rich materials) produced by industrial and
combustion processes. They classified carbon ion distribu-
tions of these samples into three categories, including low
(C1+-C5+), mid (C6+-C29+), and fullerene (greater than C30+)
carbons. Based on laboratory experiments with six types of
rBC samples generated from combustion sources, Corbin
et al. (2014) [41] reported that the C1+/C3+ ratio in the low
carbon ion category could be applied to predict whether higher
carbon ions (greater than C5+) were present. When the C1+/
C3+ ratio was close to unity, the higher carbon ions were
present. When they were absent, the ratio was less than 0.8.
Such a ratio was also proposed to be used in source
apportionment of ambient rBC aerosols which are in mixture
of two carbon ion categories (smaller versus greater than C5+)
[41]. In both fresh and aged soot emissions obtained from
wood-stove combustion experiments, Corbin et al. (2015)
[42] observed higher content of low carbon ion signals (C1+-
C3+) in flaming phase burning condition rather than the
starting phase. This could indicate that the content of low
rBC ions largely depended on combustion efficiency. The
SP-AMS fullerene ion signals could be produced by the elec-
tron ionization of pre-existing fullerene content in the sampled
rBC-containing particles [36]. In eastern China, Wang et al.
(2016) [26] firstly observed fullerene soot ions (including

80 Winter Summer Winter

60
Latitude (°)

40 Summer

20
OA, FFOA, BBOA, LO-OOA, MO-OOA
rBC, Sulfate, Nitrate, Ammonium, Chloride
0
Urban/suburban/traffic-rich
Rural/remote
-20
-150 -100 -50 0 50 100 150
Longitude (°)
Fig. 2 Locations of some recent SP-AMS measurements performed to noted that the pie charts shown here are only for the literatures that
detect ambient samples in the Northern Hemisphere during 2008–2017 presented the quantitative data about the averaged contribution of rBC-
(field campaigns time). Pie charts refer to the averaged contribution of containing particle species during the entire campaign
chemical compounds to total rBC-containing particle mass. It should be

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Curr Pollution Rep (2020) 6:440–451
C60+, C70+, etc.) from ambient air under industrial emission-
rich environment. They also estimated that industrial sector
contributed 70% to the total amount of fullerene-like ions.
Wang et al. (2018) [43] found that the low- and mid-carbon
clusters were present in similar temporal variations, which is,
however, different from fullerene ions. This indicates different
sources between low- and mid-carbon ions and fullerene car-
bon ions. Also, they quantified the relative contribution of all
measured carbon clusters and found that low-carbon ions
(91.9%) dominated the total carbon ions followed by mid
(7.6%) and fullerene carbon (0.5%) ions. By taking source
apportionment results of rBC, which was obtained from
PMF analysis with the combination of organic aerosol mass
spectra and carbon ion data, they proposed that the C1+/C3+
ratios could additionally help to distinguish ambient rBC
sources, e.g., the ratios for traffic (0.88), industry (1.29), and
cooking-related (0.01) sources [43]. Rivellini et al. (2020) [44]
integrated low- and part of mid-carbon ions (C1+-C9+) into
PMF analysis to investigate the characterization of rBC-
containing particles associated with different OA sources in
an urban environment of Singapore. They found that rBC with
higher C1+/C3+ ratios was from regional transport, which is
associated with PMF-resolved oxidized organic aerosols in-
fluenced by industrial emissions [41]. These previous studies
based on SP-ASM measurements have developed a new
methodology to study composition and sources of atmospher-
ic black carbon aerosols and improved our understanding of
refractory carbon chemistry in aerosols.
Measurements of Trace Metals
In addition to detecting soot composition, the SP-AMS tech-
nique has been also deployed to measure trace metals on soot
aerosol particles. Carbone et al. (2015) [44] have developed a
method to quantify trace metal (including Na, Al, Ca, V, Cr,
Mn, Fe, Ni, Cu, Zn, Rb, Sr, and Ba) loadings based on labo-
ratory experiments. In this method, they measured the relative
ionization efficiency (RIE) value for each trace metal, which is
the key point to determine the mass concentrations of these
trace metals. Carbone et al. (2015) [44] applied those mea-
sured RIE values and subsequently well quantified the mass
concentrations of Ba, V, and Fe observed at an oil-fired
heating station in Helsinki. Meanwhile, they also identified
the evidence of measurable metal oxides and metallic salts
by SP-AMS. Corbin et al. (2018) [45] quantified the mass
concentration of five trace metals (including V, Ni, Fe, Na,
and Ba) in BC-containing particles from heavy fuel oil com-
bustion produced by a marine diesel engine. They found that
less than 3% of the total trace metals in fine aerosols (PM2.5)
was associated with BC-containing particles and observed that
the V/Ni ratio was a 4–25 times higher in soot particles than in
total PM2.5. Given that such an enrichment of V in soot
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443
particles was not depending on soot formation process, this
metal—mainly present in smaller size particles—is therefore
suggested having higher toxicity risk for health impact.
Saarikoski et al. (2017) [46] investigated trace metals in the
bus emission particles produced from 23 individual city buses
in Helsinki, Finland. The total 15 trace metals (i.e., V, Cr, Al,
P, Mn, Ni, K, Sr, Cd, Cu, Fe, Zn, Na, Ba, and Zr) were
detected by SP-AMS. Among these trace metals, the concen-
tration of K was the largest, followed by Zn, Na, Fe, and P.
They also found bus-type dependence of the trace metals, with
the largest concentrations detected for the Euro III buses
followed by the Euro IV and EEV-EGR-DPF buses [46]. In
ambient air, Rivellini et al. (2020) [44] conducted the SP-
AMS to characterize the sources of trace metals (including
Na, K, V, Ni, and Rb) in soot aerosols in an urban environ-
ment of Singapore. Based on the V/Ni ratio analysis, they
found that the two metal ions were originated from ship emis-
sions and/or industrial heavy oil combustion in the atmo-
sphere. A good correlation between Na and rBC was ob-
served, highlighting the importance of anthropogenic emis-
sions in the formation of total particulate sodium [47]. They
also observed a possible source mixture between regional
transport of coal-fired power plant emissions and biomass
burning plumes for the metal ions Rb and K [47]. Overall,
these studies have developed and/or applied such a new SP-
AMS technique to detect trace metals, which have improved
our understanding in this research field.
Chemical Composition and Sources
of NR-PMbulk
Chemical composition of NR-PMbulk in the atmosphere was
widely measured by numerous studies with different versions
of the aerodyne AMS over the world during the last two de-
cades [15–18, 48]. Same as AMS, the SP-AMS can also mea-
sure non-refractory composition for bulk aerosols. The non-
refractory composition obtained from direct SP-AMS mea-
surement includes organic matter, sulfate, nitrate, ammonium,
and chloride. Specially, the organic aerosol spectral matrices
of the SP-AMS can be analyzed by receptor models, e.g.,
PMF [35], to further identify and quantify different OA com-
position factors from different sources and atmospheric pro-
cesses. Most SP-AMS measurements to determine the NR-
PMbulk chemistry were conducted in eastern China. This sec-
tion summarizes some results and findings using online and
offline SP-AMS measurements with the standard vaporizer
mode.
As reported by previous studies, the measurements of NR-
PMbulk chemical composition were often deployed via online
and offline detecting approaches. For example, Wang et al.
(2016) [27] firstly conducted the SP-AMS in China to inves-
tigate aerosol characteristics in urban Nanjing in Yangtze
444
River Delta during springtime in 2016. They found that or-
ganic aerosols accounted the largest fraction (45%) for the
total submicron aerosol (PM1) mass, followed by sulfate
(19.3%), nitrate (13.6%), ammonium (11.1%), rBC (9.7%),
and chloride (1.3%). Meanwhile, source apportionment of
OA using PMF analysis identified four source factors, includ-
ing two POA factors, i.e., hydrocarbon-like/traffic-related OA
(HOA) and cooking OA (COA), and two SOA factors, i.e.,
semi-volatile oxygenated OA (SV-OOA) and low-volatile ox-
ygenated OA (LV-OOA) [27]. The contributions to the total
OA mass from these factors were HOA (27.6%), COA
(16.9%), SV-OOA (27.4%), and LV-OOA (28.1%), respec-
tively [27]. In winter, Wu et al. (2018) [49] reported that
secondary inorganic aerosols, including sulfate (23.3%), ni-
trate (24.2%), and ammonium (16.9%), dominated the major
fraction of PM1 in suburban Nanjing. The SOA factors were
the most abundant compound in OA, accounting for 49% of
its total mass. Overall, these contributions of these chemical
compositions obtained from SP-AMS measurements are over-
all comparable with the standard AMS measurements over the
Yangtze River Delta region, as recently summarized by Zhou
et al. (2020) [18]. Offline SP-AMS analysis techniques, i.e.,
detecting aqueous extracts from sampled aerosol filters, were
applied in measurements of ambient aerosol chemical compo-
sition, which were mainly conduced in Eastern China. For the
first time, Ye et al. (2017) [31] conducted offline SP-AMS
measurements to investigate chemical properties of water-
soluble organic aerosol for ambient PM2.5 samples collected
in Changzhou, China. Four water-soluble OA factors, includ-
ing two POA factors, i.e., a nitrogen-rich HOA (NHOA) and a
local POA (LOA), and two SOA factors i.e., a less oxidized
oxygenated OA (LO-OOA) and a more oxidized oxygenated
OA (MO-OOA), were resolved using PMF analysis [31],
which presented evident seasonality, along with annual con-
tributions by LOA (31.2%), MO-OOA (29.7%), NHOA
(23.9%), and LO-OOA (15.3%). With the same offline SP-
AMS analysis as Ye et al. (2017) [31], Ge et al. (2017) [30]
reported five SP-AMS PMF OA factors with three POA fac-
tors, including HOA, COA, and biomass burning OA
(BBOA), and two SOA factors (i.e., LO-OOA and MO-
OOA) in urban Yangzhou, China. They found that the SOA
factors dominated the mass concentration of water-soluble
organic matter (68.1%). Overall, all of these results above,
obtained from online and offline SP-AMS measurements,
could support that fine aerosol pollution was driven by atmo-
spheric chemical and physical processes of secondary aerosols
in Eastern China, which could play an important role in for-
mation of regional haze in China.
Recently, offline SP-AMS analysis was applied in studies
of chemical properties of light-absorbing organic aerosol, so-
called brown carbon (BrC). Chen et al. (2018) [32] reported
that light absorption coefficient at 365 nm of water-soluble
organic carbon (b abs-wsoc-365nm ) presented a positive
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Curr Pollution Rep (2020) 6:440–451
correlation with oxidation state (OSc) of water-soluble brown
carbon (BrCws) among most seasons, but expect in winter, in
Nanjing of Yangtze River Delta, China. This suggests impor-
tance of secondary and/or more oxidized BrCws in contribut-
ing to aerosol light absorption at near ultraviolet wavelengths.
In addition, they found that mass absorption efficiency
(MAEws-BrC) of BrCws decreased with increased oxidation
state OSc in winter. Consistently, Chen et al. (2020) [50] also
observed a negative relationship between MAEws-BrC versus
OSc during cold months in Yangzhou of Yangtze River Delta,
China. These results indicated the role of photo-bleaching
effect due to chemical aging of BrCws in aerosol light-
absorption properties. In both the studies [32, 50], they also
found that nitrogen-containing organics could be an important
source for ambient BrC chromophores, resulting from the
positive relationship between babs-wsoc-365nm and MAEws-BrC
with the nitrogen-to-carbon (N/C) ratios and nitrogen-
containing ions, respectively. Based on PMF analysis of
water-soluble organic aerosol, Chen et al. (2020) [50] found
substantial contributions of LO-OOA (33.8%) and BBOA
(23.7%) factors to babs-wsoc-365nm in Yangzhou during cold
seasons. These studies do not only improve our knowledge
on optical and chemical properties of water-soluble brown
carbon, but they also presented such important applications
of the offline SP-AMS technique in study of atmospheric
aerosol science.
The offline or semi-online SP-AMS measurements were
also applied for a series of aqueous-phase SOA (aqSOA) stud-
ies [51–55]. Chen et al. (2020) [51] performed the SP-AMS
measurements to investigate triplet excited states (3C·)-in-
duced oxidation of 4-ethylguaiacol via aqueous-phase pro-
cesses under the laboratory simulated experiment conditions
(e.g., sunlight and ultraviolet light irradiations). They ob-
served that the oxidation state degree of aqSOA was deter-
mined by reaction time and proposed that 3C·-induced oxida-
tion might be attributed to reactions by reactive oxygen spe-
cies (3C· and 1O2) [52]. Ye et al. (2019) [54] performed
aqueous-phase reaction experiment to systemically investigate
a typical biomass-burning aqSOA compound formed via pho-
tochemical oxidation of 4-ethylphenol. They found that the
aqSOA with stronger light absorptivity at visible wavelength
could be associated with 4-ethylphenol oxidation by the or-
ganic 3C·. Liu et al. (2020) [53] did a similar aqueous-phase
reaction experiment to investigate aqueous oxidation of
dibenzothiophene, one of the typical intermediate-volatility
organic compounds (IVOCs). They observed that substantial
increase in oxidation state degree of aqSOA was attributed to
hydroxyl radical (OH) photo-oxidation, but not during the
dark oxidation [53]. Moreover, they demonstrated that OH-
initiated photochemical reactions may be a more important
secondary formation pathway to yield the light-absorbing
aqSOA with stronger absorptivity rather than 3C·-initiated ox-
idation [53]. Combining SP-AMS with gas chromatography-
Curr Pollution Rep (2020) 6:440–451
mass spectrometry (GC-MS) measurements, Ye et al. (2020)
[52] investigated aqueous-phase oxidation of three biomass
burning phenolic compounds (including 4-methylsyringol,
eugenol, and 2,4,6-trimethylphenol) induced by OH oxidation
process. Significant production of organic acids was observed
associated with the large fraction of aqSOA yields [52].
Meanwhile, they also found that light-absorbing aqSOA was
produced during the aqueous-phase process [52]. Overall,
those previous studies by using SP-AMS measurements have
improved our understanding in formation mechanisms of
aqSOA that plays an important role in affecting regional air
quality and climate.
Mixing State and Light Absorption Properties
of rBC-Containing Particles
The importance of BC aerosols to climate effect has been
established by both modeling and observation studies. BC
aerosols may be one of the strongest climate warming com-
pounds after CO2 globally [8]. However, the warming effect
for global BC, in terms of direct radiative forcing, still spans a
large range from around 0.2 to 1 W m−2 [56]. Such poorly
constrained range of direct radiative forcing for BC aerosols
could make a grand challenge in global climate change study.
BC solar radiative absorption became a key issue in climate
impact research [8], since there is still a large uncertainty in
quantification of absorptivity of BC-containing particles. It
has been well-known that absorption properties of BC aero-
sols are largely influenced by mixing states. Generally, these
mixing states can include external mixture (a BC particle is
distributed from other aerosols), internal mixture (incorporat-
ed within them), or core-shell mixture (a coated BC core by a
well-mixed shell). The chemical mixing state of BC-
containing particles has been investigated by some previous
field SP-AMS measurements at different locations (see Fig.
2). This section summarizes recent studies about mixing state
of rBC-containing particles measured by SP-AMS and corre-
sponding impact on BC light absorption.
Mixing State and Aging
The SP-AMS techniques can directly measure mass-resolved
mixing state of BC-containing particles, as described in “SP-
AMS Description”. The SP-AMS mass ratio of non-refractory
coating materials to refractory BC core (RBC = [NR-PMBC]/
[rBC]), so-called relative coating thickness, has been well ap-
plied as a proxy to examine mixing state degree of BC-
containing particles [23, 25, 29, 57]. The different range of
the RBC values was observed in different regions and seasons,
e.g., ~ 0.4–> 20 in California (urban) [23] in summer, ~ 1.8–~
14 in Fontana (near highway) in summer [25], 2.5–13.5 over
the Tibetan Plateau (4730 m a.s.l) in summer [29], 2.5–7.2 in
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445
Beijing (urban) in winter [28], 0.8–4.7 in Detling (rural) in the
UK in winter [57]. Indeed, the mixing state and coating thick-
ness of rBC-containing particles are determined by different
sources and environment conditions. A lack of coatings, cor-
responding to relatively smaller R BC value, for rBC-
containing particles was also observed in traffic-rich plumes
at different locations, such as the R/V Atlantis near California
[23, 40], Fontana [25, 39], Detling [57], London [58],
Manchester [59], and Beijing [28]. These results observed
from ambient air are well consistent with the physical charac-
terization of thinly coated BC-containing particles generated
from fresh traffic emissions in laboratory combustion experi-
ments [59]. Substantial influence of biomass burning source
on mixing state of BC-containing particles was observed from
ambient samples [29, 57–59], which could lead to thicker
coating thickness (i.e., larger RBC ratios). In laboratory wood
combustion experiments, Corbin et al. (2015) [42] observed
that the refractory oxygenated organic fragment ions (rCOn+)
were strongly associated with the refractory carbon ion signals
(Cn+). Meanwhile, they also found that the degree of BC sur-
face oxidation was not determined by burning conditions, e.g.,
either fresh or aged aerosols. These results could highlight the
important formation of oxygenated coating materials of rBC-
containing particles in both fresh and aged biomass burning.
This also might be one of the reasons to explain the rapid
oxidation processes of BC particles in biomass burning, lead-
ing to thicker coating thickness. Ahern et al. (2016) [60] in-
vestigated effect of SOA coatings, which was formed via α-
pinene ozonolysis, on the morphology of biomass-burning
soot particles with laboratory chamber experiment. They
found that dynamic shape factor of the soot particles became
from more fractal-like (nascent soot) into more spherical
(SOA-coated soot) with increasing SOA coatings. In the
Tibetan Plateau region, where it is influenced by transported
biomass burning but negligible by traffic emissions, Wang
et al. (2017) [29] observed that BBOA governed the RBC
variation of BC-containing particles during the pre-monsoon
period.
The secondary coating material transformation and BC ag-
ing play an important role in modification of mixing sate of
BC-containing particles [56]. Cappa et al. (2012) [23] and Lee
et al. (2017) [25] performed SP-AMS measurements to inves-
tigate mixing state of BC aerosols in urban environments in
California. They found that the RBC increased with photo-
chemical age, which was estimated by the –log([NOx]/
[NOy]) ratio. Moreover, the secondary coating materials, i.e.,
oxygenated organic aerosol (OOA) and sulfate, of BC-
containing particles presented a positive relationship with at-
mospheric photochemical aging [23, 25]. In an urban environ-
ment (Toronto), Lee et al. (2015) [24] observed that rBC aero-
sols in accumulation-mode particles were substantially mixed
with secondary components and indicated that these rBC-
containing particles were chemically aged. At a rural site
446
(Detling) in the UK, Liu et al. (2015) [57] also observed in-
crease trends in secondary coating materials (OOA and ni-
trate) as increasing of RBC and oxidation state of rBC-
containing particles during wintertime, indicative of influence
of photochemical aging processes on mixing state of BC aero-
sols. In the Tibetan Plateau region (4730 m a.s.l), Wang et al.
(2017) [29] found that the secondary coating materials
(including LV-OOA, sulfate, nitrate, and ammonium) of
rBC-containing particles were predominantly linked to photo-
chemical productions during a monsoon season. In wintertime
Beijing, Wang et al. (2019) [28] observed that the fraction of
secondary coating materials and oxidation state of rBC-
containing particles increased as the RBC increase during pol-
luted period, highlighting the substantial contribution of the
chemical aging process to the heavy haze pollution. Based on
mixing state and cluster analysis of single particle measured
by SP-AMS in summertime Fontana, USA, Lee et al. (2019)
[39] found that the freshly formed SOA near traffic emission
source could enhance the homogeneity of atmospheric rBC-
containing particles. Based on SP2 measurements in Beijing
(summer and winter), Liu et al. (2019) [61] firstly performed
source apportionment of BC particles by different classifica-
tions of coating thickness and BC core size, including small,
large uncoated, moderately coated, and thickly coated rBC
particles, respectively. By the combination of results obtained
from the SP2-method and the SP-AMS PMF-resolved rBC
sources, they found that thickly coated rBC-containing parti-
cles were mainly associated with LV-OOA coatings, whereas
small or large uncoated BC were from primary traffic and
biomass burning emissions, respectively [61]. These results
could suggest a significant role of aged SOA formation in
the transformation of thickly coated rBC particles in urban
environments. Overall, these results above could make signif-
icant implications for understanding influence of aerosol
mixing state on absorption properties of BC-containing parti-
cles in different ambient environments. The next section will
discuss the relation between mixing state of BC aerosols and
aerosol light absorption properties.
Effect of Mixing State on BC Radiative Absorption
Radiative absorption of BC with internal mixture is substan-
tially greater than that with external mixture. This is due to the
fact that coatings of internally mixed BC-containing particles
focus more photons onto the BC core (so-called lensing ef-
fect), which leads to BC absorption enhancement (Eabs) [62,
63]. The magnitude of BC absorption enhancement can span
from negligible up to a factor of more than 3. Thus, such
enhancement effect could make more than 200% uncertainty
in direct radiative effect of atmospheric BC aerosols. Despite
many recent studies focused on quantitative assessment of
Eabs, a detailed parameterization solution to simulate Eabs
has not been actually well resolved in climate models. In
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Curr Pollution Rep (2020) 6:440–451
practice, most models simply estimate Eabs by around 50%
enhancement for BC radiative absorption globally [64]. The
magnitude of Eabs is determined by sources, mixing state, and
atmospheric aging of BC-containing particles [56]. Some pre-
vious studies at different geographic locations have focused
on investigating the relationship of Eabs versus mixing state
and atmospheric aging of BC-containing particles.
Based on observational constraints obtained from SP-AMS
measurements in an urban environment in California, Cappa
et al. (2012) [23] reported that Eabs theoretically simulated
with core-shell model was gradually increased as a function
of RBC. However, this simulated result is largely different
from direct measurement showing a lack of E abs [23].
Similarly, such limited dependence of Eabs on RBC—even up
to the RBC ratios of 5 during wintertime (in Fresno, CA) or of
10 during summertime (in Fontana, CA)—was also observed
in the two cities [65]. These observations demonstrate that
lensing-induced Eabs could be very small and even negligible
in relatively near primary traffic-rich emission environments.
This could be also associated with many field [57, 66] and
laboratory [59] measurements, indicating a lack of Eabs for
BC-containing particles from fresh traffic emissions. As re-
ported by a very recent study [67], lower-than-expected en-
hancements in ambient measurements could be explained by a
combination of two factors: (1) overestimated absorption of
internally mixed BC with core-shell model (i.e., a standard
spherical-concentric model) and (2) inadequate consideration
of heterogeneity in particle-to-particle composition.
At a rural site in the UK, Liu et al. (2015) [57] observed an
evident increase of Eabs as a function of RBC. This relationship
between observed Eabs and RBC was well-simulated by Mie
theory models along with observational constraints, suggest-
ing that the magnitude of mixing-induced Eabs was strongly
depending on BC coating amount. Moreover, they also ob-
served that the size of BC core was increased as a function of
RBC and carbon oxidation state, respectively. This indicates
that photochemical aging processes generated significant pro-
duction of non-refractory coatings (i.e., OOA and nitrate) and
growth of BC-containing particles [57]. In the Tibetan Plateau
(4730 m a.s.l), Wang et al. (2017) [29] first observed a posi-
tive relationship between Eabs and RBC, which was attributed
to the major influence of transported BBOA coatings. From
laboratory biomass-burning experiments, McMeeking et al.
(2014) [68] also observed large absorption enhancements for
RBC greater than 10. Tasoglou et al. (2015) [69] performed
smog chamber experiments and demonstrated that Eabs could
be observed in aged smoke (i.e., exposed to UV light, ozone,
or OH radicals), in which substantial secondary organic ma-
terials condensed on the preexisting particles. In addition, they
also found a consistent Eabs between observed and predicted
with core-shell model only for the aged particles, which is
consistent with a long-term field measurements in urban back-
ground region of Paris [70]. In a highly polluted environment
Curr Pollution Rep (2020) 6:440–451
(Beijing) during winter, Xie et al. (2019) [71] found that Eabs
increased with the RBC increasing and the oxygen to carbon
(O/C) ratio of BC-containing particles, respectively.
Meanwhile, decrease trends in primary organic aerosols
(fossil-fuel OA and BBOA) and increase trends in secondary
compounds (LV-OOA, nitrate, and sulfate) were also ob-
served as increase of R BC , respectively. These results
highlighted significant secondary coating formation during
BC aging. In summer Beijing, Eabs was also observed strongly
depending on the RBC mass ratio, which was increased as
increase of photochemical age along with substantial second-
ary formation of nitrate, sulfate, and aged SOA [72]. In
Nanjing, Ma et al. (2020) [73] highlighted that the formation
of particulate ammonium nitrate associated with traffic emis-
sions could have significant impact on BC aging and Eabs in
urban environments during summertime. In urban plumes in
Northwestern Europe, Eriksson et al. (2017) [74] observed the
rapid diesel soot aging, i.e., from fresh to aged soot, caused by
secondary ammonium nitrate formation and water uptake un-
der cold dark and high humidity environment conditions.
Based on laboratory simulation experiments, Yuan et al.
(2020) [75] demonstrated that the morphology of BC particles
could be restructured from fractal to near-spherical shapes by
increasing secondary ammonium nitrate coating, which result-
ed in increasing of Eabs. All these findings above suggested
that the secondary coating material formation plays an impor-
tant role in amplification of radiative effect induced by inter-
nally mixed BC aerosols in the atmosphere.
Future Perspectives
In this review, we summarized recent SP-AMS measurements
and corresponding results and findings, including characteri-
zation of carbon cluster ions, trace metals, chemical composi-
tion and sources of non-refractory aerosols, and mixing state
and radiative absorption properties of rBC-containing parti-
cles. These previous studies have made significant progresses
in understanding aerosol chemistry and physics in the atmo-
sphere and have also provided some observational constrains
in aerosol modeling studies. Based on these studies, we pro-
pose some potential future work that would be done with SP-
AMS measurements, as follows:
(1) Long-term SP-AMS measurements. Air pollution and
climate change issues caused by atmospheric aerosols
have been well recognized, especially in the highly pol-
luted regions with intense anthropogenic emissions, e.g.,
eastern Asia. In order to mitigate air pollution and cli-
mate, some countries (e.g., China) have implemented
very strict emission reduction actions during the last de-
cade [76–78] and planed future emission targets [79].
However, it is still a great challenge to fully address the
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447
response of aerosol chemistry to the change of emis-
sions, which could limit the precise formulation of emis-
sion control policies. This is mainly due to a lack of long-
term measurements of aerosol chemical composition in
the atmosphere. As SP-AMS can provide highly time-
resolved aerosol chemical composition, its long-term
measurements can be conducted to investigate year-
round temporal trends in secondary aerosols and their
gas-phase precursor emissions, as well as their nonlinear
relationship (e.g., SOA versus volatile organic com-
pounds). Meanwhile, influence of future emission con-
trol on interactions between anthropogenic and biogenic
sources on aerosol chemistry could be studied in some
typical biogenic-rich and biogenic-poor environments,
e.g., Southeastern USA [80] and Eastern China [81],
respectively. In addition, in situ long-term measurements
could also provide sufficient data for capturing the year-
round cycles of air pollution episodes, for instance in
winter Beijing [82] and in winter/spring Paris [83],
which could be used to investigate formation mecha-
nisms of aerosol-induced air pollution. Furthermore,
feedbacks of further emission control on the chemistry
and sources of rBC-containing particles could be special-
ly studied by long-term SP-AMS measurements.
(2) Multi-site measurements. Multi-site measurements are of
great importance to provide spatial characterization of
aerosol chemical composition and sources, especially in
highly polluted regions and/or seasons [84, 85].
Although aerodyne standard AMS measurements have
been widely deployed at numerous sites over the world
to investigate the chemistry and sources of NR-PMbulk in
the past years, the study on the chemical composition,
mixing state, and sources of rBC-containing particles
measured by SP-AMS is still very limited. For example,
it was demonstrated that BC catalytic chemistry played a
predominate role in ambient sulfate aerosol formation,
which could facilitate regional haze formation in
Beijing [86]. However, such a BC-catalyzed sulfate for-
mation pathway is missed within aerosol chemistry
transport models, which may make some uncertainties
in evaluating impact of aerosols on air quality and radi-
ative forcing. It is essential to further investigate such
BC-catalyzed chemistry mechanism under different en-
vironment conditions in other regions by using SP-AMS
measurements, particularly in relatively large SO2 emis-
sion regions, like China and India. The mixing state of
BC-containing particles is largely influenced by primary
BC sources [59] and secondary formation of coating ma-
terial on BC particles in the atmosphere [23, 25, 39]. It is
essential to understand differences of aerosol chemistry
between NR-PM1 and NR-PMBC particles at more dif-
ferent sites over different regions. In addition, source
apportionment and chemical evaluation of SP-AMS
448
rBC-containing particles (including NR-PMBC and trace
metals in soot) could be further performed at different
sites over different regions to understand spatial charac-
terization of sources and atmospheric aging processes of
internally mixed BC aerosols.
(3) Offline SP-AMS measurements. In practice, it could not
avoid high costs of instrument maintenance, which
brings a great challenge for multi-site or long-term on-
line SP-AMS measurements. Off-line filter analysis has
been well applied in laboratory SP-AMS measurements
[30–32, 50, 87], which provided a way to investigate
horizontal distributions of water-soluble aerosol species
and sources. This off-line SP-AMS method—which is
less cost rather than online method—could be further
performed to detect more samples collected at more typ-
ical sites (e.g., rural, suburban, urban, urban background,
etc.) in different countries/regions/cities over the world
during a same sampling period. However, the limited
time resolution (e.g., generally 24 h) of off-line data
brings a challenge to further understand evolution pro-
cesses of aerosol particles in the atmosphere. In addition,
off-line analysis seems not available to detect mixing
state of rBC-containing particles. Regarding these points,
it would be helpful to develop a compact version of the
SP-AMS that is more appropriate for purposes of multi-
site and even long-term measurements only for chemical
composition of rBC-containing particles in the future.
(4) Mixing state, chemical aging, and radiative absorption.
Eabs is largely influenced by mixing state, sources, and
aging of rBC-containing particles in the atmosphere.
Dynamic changes in coating materials against Eabs have
been often observed at some sites [29, 57]. It would be
interesting to explore relationship between mixing state
and aging of BC-containing particles and Eabs by using
SP-AMS measurements in environmental chamber ex-
periments in different regions. The SP2 can provide
physical properties of BC particles, including relative
coating thickness and size distribution of BC core. By
using the SP2 source apportionment method, the rBC
aerosol sources associated with different coating thick-
ness clusters could be identified and quantified [61]. The
SP-AMS PMF analysis of mass spectra can be applied to
quantify chemical-tracer-based sources of rBC-
containing particles [23, 25, 28, 38]. The combination
of these SP2 and SP-AMS methods can provide new
insights into further understanding more detailed mixing
state, sources, and chemical evolution of ambient BC
aerosols. Furthermore, such combined source apportion-
ment method, coupled with measurements of aerosol op-
tical properties, could be also applied to further investi-
gate source-dependent optical properties and aging of
rBC-containing particles in the atmosphere. In addition,
understanding of vertical-resolved relationship between
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Curr Pollution Rep (2020) 6:440–451
mixing state of rBC-containing particles and Eabs is very
limited, which could be investigated by aircraft measure-
ments. This is very critical, yet reported so far to our
knowledge, to provide direct observation data to under-
stand the vertical characterization and to constrain aero-
sol radiative transfer models.
(5) Mixing state and hygroscopic properties. The role of BC
in acting as CCN is depending on hygroscopicity of BC-
containing particles. Hygroscopic properties of BC-
containing particles are controlled by mixing state and
corresponding coating materials. More hydrophilic coat-
ing materials lead to high hygroscopicity of BC-
containing particles. Based on hygroscopicity tandem
differential mobility analyzer (HTDMA) and SP-AMS
measurements in the UK, Liu et al. (2013) [88] found
that internally mixed rBC particles present different hy-
groscopic properties for less- and more-hygroscopic
coating compounds, respectively. The growth factor of
rBC-containing particles was highly influenced by the
coating material of ammonium nitrate, whereas SOA
suppressed their growth factor. In eastern China, Wu
et al. (2019) [89] found that secondary inorganic and
more oxidized organic coatings may govern the magni-
tude of hygroscopicity parameter of rBC-containing par-
ticles in the atmosphere. However, a lack of SP-AMS
measurement has been applied in the study of BC aerosol
hygroscopicity. Given the large uncertainties of impact
of BC aerosols on droplet size, lifetime, formation of
cloud, and wet precipitation, it is essential to further in-
vestigate chemical/size-resolved hygroscopic properties
of BC-containing particles by using SP-AMS coupled
with HTDMA measurements in more different environ-
ments and regions. Aircraft measurements could be also
applied in this subject study to characterize the vertical
and horizontal distributions of hygroscopic properties of
BC aerosols, as well as to measure samples in cloud,
especially in highly polluted regions, such as eastern
Asia and south Africa.
Funding This work was supported by the National Key Research and
Development Program of China (No. 2018YFC0213802) and the
National Science Foundation of China (21777073).
Compliance with Ethical Standards
Conflict of Interest The authors declare that they have no conflict of
interest.
Human and Animal Rights and Informed Consent This article does not
contain any studies with human or animal subjects performed by any of
the authors.
Abbreviations AMS, Aerodyne aerosol mass spectrometer; Q-AMS,
Quadrupole aerosol mass spectrometer; C-ToF-AMS, Compact time-of-
flight aerosol mass spectrometer; HR-ToF-AMS, High-resolution time-
Curr Pollution Rep (2020) 6:440–451
of-flight aerosol mass spectrometer; SP-AMS, Soot particle aerosol mass
spectrometer; SP2, Single-particle soot photometer; HTDMA,
Hygroscopicity tandem differential mobility analyzer; RIE, Relative ion-
ization efficiency; MAAP, Multi-angle absorption photometer; CCN,
Cloud condensation nuclei; IN, Ice nuclei; BC, Black carbon; rBC,
Refractory black carbon; PM 2.5 , Fine particulate matter; PM 1 ,
Submicron particulate matter; NR-PMbulk, Bulk non-refractory particu-
late material; NR-PMBC, Non-refractory particulate material of BC-
containing particles; R-PMBC, Refractory particulate material of BC-
containing particles; RBC, Mass ratio of NR-PMBC to rBC core; Cn+,
Carbon cluster ions; rCOn+, Refractory oxygenated organic fragment
ions; PMF, Positive matrix factorization; OA-, Organic aerosol; POA,
Primary OA; SOA, Secondary OA; FFOA, Fossil-fuel OA; HOA,
Hydrocarbon-like/traffic-related OA; NHOA, Nitrogen-rich HOA;
BBOA, Biomass burning OA; COA, Cooking OA; LOA, Local POA;
OOA, Oxygenated OA; SV-OOA, Semi-volatile OOA; LV-OOA, Low-
volatile OOA; LO-OOA, Low oxidized OOA; MO-OOA, More oxidized
OOA; N/C , Nitrogen-to-carbon ratio; O/C, Oxygen-to-carbon ratio; OSc,
Oxidation state of carbon; WSOC, Water-soluble organic carbon; BrC,
Brown carbon; BrCws, Water-soluble BrC; babs-wsoc-365nm, Light absorp-
tion coefficient of WSOC at wavelength 365 nm; MAEws-BrC, Mass ab-
sorption efficiency of BrCws; Eabs, Light absorption enhancement of BC-
containing particles
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