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Quantifying the Light-Absorption Properties and Molecular

Composition of Brown Carbon Aerosol from Sub-Saharan African
Biomass Combustion
Vaios Moschos,* Cade Christensen, Megan Mouton, Marc N. Fiddler, Tommaso Isolabella,
Federico Mazzei, Dario Massabò, Barbara J. Turpin, Solomon Bililign,* and Jason D. Surratt*
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ABSTRACT: Sub-Saharan Africa is a hotspot for biomass burning (BB)-derived carbonaceous aerosols, including light-absorbing
organic (brown) carbon (BrC). However, the chemically complex nature of BrC in BB aerosols from this region is not fully
understood. We generated smoke in a chamber through smoldering combustion of common sub-Saharan African biomass fuels
(hardwoods, cow dung, savanna grass, and leaves). We quantified aethalometer-based, real-time light-absorption properties of BrC-
containing organic-rich BB aerosols, accounting for variations in wavelength, fuel type, relative humidity, and photochemical aging
conditions. In filter samples collected from the chamber and Botswana in the winter, we identified 182 BrC species, classified into
lignin pyrolysis products, nitroaromatics, coumarins, stilbenes, and flavonoids. Using an extensive set of standards, we determined
species-specific mass and emission factors. Our analysis revealed a linear relationship between the combined BrC species
contribution to chamber-measured BB aerosol mass (0.4−14%) and the mass-absorption cross-section at 370 nm (0.2−2.2 m2 g−1).
Hierarchical clustering resolved key molecular-level components from the BrC matrix, with photochemically aged emissions from
leaf and cow-dung burning showing BrC fingerprints similar to those found in Botswana aerosols. These quantitative findings could
potentially help refine climate model predictions, aid in source apportionment, and inform effective air quality management policies
for human health and the global climate.
KEYWORDS: smoldering combustion, aethalometer, mass-absorption cross-section, emission factors, hierarchical clustering

1. INTRODUCTION based guidelines by a factor of up to 30.8 African BB-derived

Africa contributes a majority of the global annual atmospheric
carbonaceous aerosol (CA) mass from biomass burning (BB)
emissions, where CA is the sum of particulate organic and
elemental carbon.1 BB aerosols persist throughout the
Southern Hemisphere’s wintertime,2 influencing the climate
via aerosol-radiation and aerosol-cloud interactions.3,4 In sub-
Saharan Africa, the main BB-derived CA sources are residential
solid fuel combustion, prescribed fires, and wildfires,
particularly in the Congo Basin, west Africa, and southern
African savanna grasslands.5,6 Solid fuels are used for over two-
thirds of household energy consumption in most sub-Saharan
African countries,7 leading to indoor and outdoor air pollution
levels that often exceed the World Health Organization health-
CA is likely to increase with the projected population growth
and urbanization, due to widespread poverty and limited clean
energy access.9,10
Brown carbon (BrC), a subset of light-absorbing organic
carbon in CA, is a critically important yet poorly understood
Received: November 9, 2023
Revised: January 19, 2024
Accepted: January 22, 2024

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A Environ. Sci. Technol. XXXX, XXX, XXX−XXX
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component of BB aerosols emitted from solid fuels during
smoldering combustion in both natural and residential
sectors.11−13 The positive direct radiative forcing of BB-
derived BrC aerosols in subtropical Africa varies considerably,
yet it potentially matches the cooling effect of nonabsorbing
organic aerosols (OAs).14 Common reasons for negative
model bias15 in the CA warming effect in southern/sub-
Saharan Africa are the neglect of light absorption by BrC
aerosols16−18 and the scarcity of observational BrC data.19−22
In addition, BrC aerosol degrades visibility and CA poses
human health risks upon inhalation,23,24 including increase in
noncommunicable diseases.25
Despite its well-recognized impacts, a comprehensive
analysis of the complex molecular-level composition and
optical properties of (sub-Saharan Africa) BB-derived BrC-
containing aerosol remains elusive.26,27 Accurate quantification
of individual BrC species by mass and determination of their
emission factors (EFs) pose substantial challenges.28,29 While
numerous BrC species and their contributions to absorbance
have been identified upon solvent extraction, the use of an
extensive array of standard compounds for mass quantification
was previously deemed impractical.28,30 Additionally, the
absorptivity of OAs31 and the relative contributions of
individual species to BrC (or total aerosol) mass are expected
to vary with the specific emission source, combustion
efficiency, and atmospheric conditions/processing (i.e., phase
partitioning, oxidation, and aging).13,32−34 Crucially, a system-
atic correlation between the molecular-level composition of
primary/aged BrC and broad-band optical absorption proper-
ties of OAs in the particle phase is currently lacking.35
To fill these knowledge gaps, we conducted smog chamber
experiments using a range of African biomass fuels that
simulate smoldering combustion36 and atmospherically
relevant relative humidity (∼65% RH). We quantified the
real-time optical absorption properties of the generated
organic-rich aerosols and examined their dependence on the
fuel type, RH, and (photochemical) aging conditions. Using an
optimized chromatographic separation protocol and a
comprehensive suite of BrC authentic standards, we analyzed
filter-collected aerosols for molecular-level absorbance and
chemical composition. Furthermore, we correlated the light-
absorption properties with the molecular-level composition of
the chamber-generated BrC aerosol species and assessed their
atmospheric relevance by analyzing airborne particulate matter
(PM) collected at two locations in Botswana in the winter.
2. MATERIALS AND METHODS
2.1. Sub-Saharan African Biomass Fuel Combustion
Chamber Experiments. We used 11 African biomass fuels,
including hardwood species (acacia, eucalyptus, mopane,
mosetlha, mukusi, wanza, and wild olive), tree branches
(from mokala) and leaves (from mopane), cow dung, and
savanna grass [Supporting Information (SI) Text S1]. Most
fuels are native to Botswana and neighboring countries mainly
in eastern and southern Africa (Figure S1) and are frequently
used for firewood in this region (Text S1).
We sampled BB primary and aged emissions using an indoor
combustion-chamber system at North Carolina A&T State
University (NC A&T)37 (Text S2). The 9 m3 Teflon chamber
was either dry (<10% RH) or conditioned to ∼65% RH before
each experiment. We combusted ∼0.4 g of each fuel (dried and
debarked) in a tube furnace that is uniformly heated at the
center over the burning region (Text S2). The ignition
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temperature was set to 450 °C, yielding smoldering-dominated
combustion (fire-average modified combustion efficiency,
MCE < 0.9; Table S1) and organic-rich38 emissions of PM2.5
(particulate matter with an aerodynamic diameter < 2.5 μm or
fine aerosol; using a cyclone, Text S2) into the dark chamber.
We defined three aerosol aging conditions within each
chamber experiment: (1) primary aerosol sampled within 30
min to 1 h of combustion, (2) dark-aged aerosol sampled 4 h
after combustion in the dark chamber, and (3) photochemi-
cally aged aerosol (following dark aging) sampled after smoke
was irradiated for 2 h with UV lamps (Text S2). No additional
oxidants, seed aerosol, or volatile organic compounds were
injected into the chamber, apart from those generated during
combustion or upon irradiation.
2.2. Aethalometer Measurements and Calibration.
We quantified the light-absorption properties of BrC-
containing OAs generated from the combustion of African
biomass fuels using a dual-spot aethalometer (AE33, Magee
Scientific). The AE33 system measures light transmission
through aerosol-loaded spots on a filter tape (I), compared to
transmission through a reference obtained by passing clean air
through a filter tape spot (Io). The AE33 simultaneously
analyzes at seven optical wavelengths (λ) from the near-
infrared (950 nm) to near-UV (370 nm). The optical
attenuation (ATNλ) is defined as ATNλ = −100 * ln(Iλ/I0,λ).
In this study, we determined the attenuation coefficient, batn,λ
(Mm−1), for optically absorbing aerosols by evaluating (see
Text S2) the light attenuation rate of change passing through a
particle-laden filter. Dynamic blanks were performed by
placing a HEPA filter at the inlet, allowing the aethalometer
to sample particle-free chamber air; we found that gases made
no contribution to ATNλ. We conducted three 10−15 min
aethalometer measurements within each experiment with one
measurement for each aging condition. We employed the
formula
batn,AE33, = D × S × ( ATN /100)/(Fin × t) (1)
where S represents the spot area, Fin is the aerosol flow rate,
and t is the time (1 min resolution; therefore, batn,AE33,λ is the
average of 10−15 values at each measurement/aging
condition). High chamber-aerosol mass concentrations (M ≈
800 μg m−3 for primary emissions) required dilution with zero
air, where the dilution ratio (D) was 10, using a dilution jar to
acquire multiple ATN values for accurate batn,AE33,λ calculations
(Text S2).
During aethalometer measurements, we simultaneously
collected 47 mm quartz fiber filters (QFFs; Whatman, QMC
fired, 1855-047), with a scrubber (Ozone Solutions, Inc.)
attached to the inlet to reduce gas-phase adsorption on the
QFFs.39 For 20 selected QFFs, we determined the aerosol
absorption coefficient (babs) with a multiwavelength absorb-
ance analyzer (MWAA)40 to determine AE33 calibration
coefficients: Cλ = babs,MWAA,λ/babs,AE33,λ; interpolation of
babs,MWAA to AE33 wavelengths was based on adjacent-
wavelength absorption Ångströ m exponents (AAE,
ln(babs, 1 / babs, 2)
AAE 1 2 = ln( 1 / 2)
) that assumed a power-law
relationship. Cλ values (dimensionless) were applied to rectify
batn,AE33 (eq 1) for apparent absorption due to scattering
artifacts, such as multiple scattering effects, where we
determine the approximate babs for all samples (babs,AE33,λ =
batn,AE33,λ/Cλ, in Mm−1) and assume that MWAA measure-
ments are closer to the true absorption value.41 Moschos et al.
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reported a largely wavelength-independent C of ∼2.3 for year-
long aerosols in Switzerland that consisted of both elemental
and organic carbon.41 However, for the chamber African BB-
OAs, we found the C values to be wavelength-dependent:
Cλ=370 nm = 4.1, Cλ=470 nm = 3.2, Cλ=520 nm = 2.9 [relative errors
(1σ/mean) ∼ 25%], and Cλ=590 nm = 2.0, with a decreasing
correction factor with increasing wavelength but no systematic
variation between fuels or aging conditions. To the best of our
knowledge, this is the first study that presents calibration
coefficients for the aethalometer batn that vary substantially
with the wavelength. This variability significantly affects babs,λ
and AAEs, compared to studies that use or assume constant
coefficients independent of wavelength and might be related to
the distinct spectral scattering properties of African BB-OAs.
We divided babs,λ by the chamber-aerosol M (based on
scanning mobility particle sizer, SMPS, measurements; Text
S2) to estimate the fine aerosol absorption cross section per
unit mass or mass-absorption cross-section (MAC, m2 g−1) of
the BrC-containing organic-rich aerosols
MAC = batn,AE33, /(C ·M )
(2)
2.3. Aerosol Filter Collection for Chemical Composi-
tion Measurements. For molecular-level BrC analysis,
Teflon filter samples (Tisch Scientific, SF18040; 47 mm
diameter, 2 μm pore size, 38 mm aerosol collection diameter)
were collected from each chamber experiment listed in Table
S1. The sampling flow rate and duration were 30 L min−1 and
10−20 min, respectively.
We also collected 47 mm Teflon filter samples at the onset
of the 2022 wintertime fire/heating season in southern Africa
(Botswana). Total suspended PM was sampled from June 24
to July 21 in Gaborone, the capital city, at a time when the PM
concentration was high (∼150 μg m−3), and at the Botswana
International University of Science and Technology (BIUST)
weather station near Palapye, which had a lower PM
concentration (campaign-average: 10 μg m−3). Ten Teflon
filter aerosol samples were collected in total, with some day/
night filters sampled over two different dates (Table S1).
Details of filter sampling (including chamber/field blanks) and
sample handling are provided in Text S2.
2.4. Molecular-Level Analysis of Chamber and
Ambient BrC Aerosols. We employed a multistage analytical
platform that combines reversed-phase liquid chromatography
(RPLC), diode array detection (DAD), and high-resolution
quadrupole time-of-flight tandem mass spectrometry (HR-
QTOFMS/MS) with electrospray ionization (ESI) operated in
both positive (+) and negative (−) modes. We analyzed
methanol extracts of 25 selected chamber and 10 ambient
Teflon filter samples (Table S1). The sample preparation
protocol and details of the RPLC/DAD-ESI-HR-QTOFMS/
MS method, including gradient elution scheme, operating
conditions, and data analysis procedures, are described in Text
S3.
2.5. Quantification of BrC Species with Standards. We
made use of 100 authentic standards (100 ppm stock solution
in methanol; 25 species/group) for quantification of BrC
species. Standard selection was based on our preliminary
molecular analysis of chromophoric species in filter samples
from test chamber burns, combined with C6−20HHO1−10N0−2
BrC formulas (tentative structures) in the literature (see the
Laskin-group papers in “References” section). ChemSpider was
used to determine if a potential (aromatic) structure would
reasonably exhibit absorption in UV. Details of the standard
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preparation and characterization are provided in Text S4. A
sample-average extracted wavelength DAD chromatogram and
the mass absorption coefficient spectra of target BrC species in
methanol solution (Text S4) are provided in Figures S2 and
S3.
Calibration curves were generated by measuring a mixture of
the 100 standards, ranging from 0.002 to 10 ppm, at the
beginning and end of sample analysis (the respective vials were
stored in a freezer during the aerosol-sample analysis). Each
standard’s response factor (RF) was determined (Text S4)
using the linear-range extracted ion chromatogram (EIC) peak
area (A) per μg mL−1. Positional isomers exhibited distinct
retention times (RTs) due to polarity differences, with their
RFs differing by a factor of up to 2 (Text S4).
Table S2 displays those standards identified with our
analytical platform and used to quantify (Text S4) the mass
of the BrC species found in the aerosol samples including the
vendor, purity, ESI RF, and fragmentation information (Table
S3). The IDs refer to the complete list of 182 BrC species
(Table S4). In Text S4, we delineate our systematic approach
to quantifying BrC species in aerosol filter samples. Briefly, for
BrC species without a matching authentic standard, we
assigned surrogate standards based on structural similarity
and adjacent RTs (Table S4). We note that during the sample
preparation drying step (Text S3), about one-third of the mass
evaporated; thus, reported results have been adjusted for
recoveries (Text S4). We discuss the strengths and limitations
of the methodology for quantification in Text S5.
2.6. Hierarchical Cluster Analysis. We applied hierarch-
ical cluster analysis to visualize the complex BrC molecular-
level composition matrix in heatmaps (Text S6). Dimension-
ality reduction through species/sample clustering assisted in
identifying: (a) similarities in BrC composition between
chamber- and ambient-aerosol filter sample extracts and (b)
potential tracer species for particular African fuel types or aging
processes.
3. RESULTS AND DISCUSSION
3.1. Light-Absorption Properties of Sub-Saharan
African Biomass Fuel-Derived OAs. 3.1.1. MAC of Primary
OAs. The light-absorption potential, expressed as the broad-
band MAC (MACλ; Section 2.2 and eq 2), of primary BB fine
aerosols from African solid fuel smoldering combustion in the
humid (∼65% RH) chamber experiments, exhibits a strong
fuel-type dependency (Figure 1). BB aerosol emissions derived
from hardwoods (acacia, eucalyptus, mopane, mosetlha,
mukusi, wanza, and wild olive) are more absorptive (0.8−1.6
m2 g−1 at 370 nm; 0.2−0.5 m2 g−1 at 470 nm) than BB aerosol
emissions from mokala branches, mopane leaves, cow dung,
and savanna grass (0.2−0.7 m2 g−1 at 370 nm; 0.1−0.2 m2 g−1
at 470 nm), as shown in Table S1. The MACOA,λ range of the
African hardwood-derived BB aerosol emissions is comparable
to, or lower than, the methanol-extractable primary particulate
BB-OA MACλ reported for ambient samples from Switzerland
(1.5−2.3 m2 g−1 at 370 nm; 0.4−0.6 m2 g−1 at 470 nm; Figure
1). The latter represents hardwoods burning in residential
stoves at European rural sites (e.g., beech, oak, and birch) and
is comparable to previously reported conventional primary BB-
OAs from lab experiments and observations in different
atmospheric environments.41 These values41 were constrained
within a narrow range by applying source apportionment on
UV−vis absorbance measurements31 combined with Mie
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Figure 1. MAC spectral range (shaded areas: min−max) for primary
organic-rich aerosols injected into the humid chamber. This was
derived from the smoldering combustion of African hardwood species
(yellow; N = 7) and other biomass fuels (blue; N = 4) and quantified
(eq 2) by using calibrated aethalometer measurements (Section 2.2).
“Other” includes savanna grass, cow dung, and tree leaves/branches.
Literature-reported ambient primary BB-OA from Switzerland41
(brown) is also shown (see Section 3.1.1).
calculations at AE33 wavelengths,41 which is a fundamentally
different approach than that applied here (Section 2.2.).
3.1.2. Absorption Emission Factors. The humid-chamber
OA absorption emission factor spectra (AEFOA,λ) were
estimated by multiplying MACOA,λ (in m2 g−1) by the PM
mass-based EF (EFPM; Text S2), since the smoldering
combustion particles are organic-rich. AEFOA values at 370
nm range from 5 (leaves) to 37 (mukusi) m2 kg−1 of fuel
burned (Table S1), with an average of 19 m2 kg−1. These
values are similar to the 25−35 m2 kg−1 range reported by
Selimovic et al. for lab-simulated Western US wildfire-derived
BrC measured at 401 nm with an MCE < 0.9.42 Furthermore,
Martinsson et al. burned logs of birch and reported AEF values
for BrC in the range of 19−24 m2 kg−1 at 370 nm.43 Tian et al.
reported BrC AEF values measured at 370 nm relevant to
China, ranging from 15−47 m2 kg−1 for crop residues.44
Notably, the AEF370 nm value for both the African savanna grass
(Table S1) and South Asian grass45 is ∼9−10 m2 kg−1. Our
AEFs decreased by a factor of 5 at 470 nm and further at 660
nm to an average of 1.7 m2 kg−1, with a range from 0.7 (leaves)
to 3.2 (wanza) m2 kg−1 (Table S1).
3.1.3. Impact of Humidity and UV Exposure on MAC. In
our chamber experiments, the MAC spectra were influenced
Figure 2. Impact of environmental conditions, simulated during smog chamber experiments, on fuel-specific MACλ. The two conditions evaluated
are (a) primary emissions in the dry versus prehumidified chamber and (b) photochemical aging of primary emissions in the humid chamber.
Eucalyptus is not featured here, because only humid-chamber primary emissions were sampled for this fuel.
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not only by the biomass fuel type (Figure 1) but also by
humidity and UV exposure (Figure 2). In primary emissions,
MAC370 nm values were up to 1.4 times higher under dry
chamber conditions (<10% RH) compared to those in a
prehumidified (∼65% RH) chamber (Figure 2a), with no
evident wavelength dependence. Interestingly, this trend was
not observed for leaves, grass, and mokala branches, which had
similar MAC370 nm values at ∼65% RH and <10% RH. Perhaps
this could be due to differences in hygroscopicity or phase
state. Section 4 discusses the uncertain role of chamber wall
losses (at varying RH conditions) of gases or particles that
might contribute to BrC. Conversely, Figure 2b highlights that
when primary emissions are aged via UV exposure in the ∼65%
RH chamber, there is a reduction in aerosol MAC by up to
25% at 370 nm (again, leaves are an exception). Yet, MAC
showed an average increase of 1.5 times in the 470−660 nm
range, with cow dung as an exception. UV light affects MAC in
two main ways: (1) By altering aerosol composition which
influences absorption, either through UV photobleaching or
UV-driven gas-phase oxidation or multiphase chemistry; 2) By
changing the aerosol mass concentration.33,46−48 The change
in MAC may occur due to secondary organic aerosol (SOA)
formation via gas-phase chemistry, in the presence of emissions
like organics, NOx, and HONO. Both photobleaching and
formation of purely scattering SOA can decrease the MAC (see
also Sections 3.2.2 and 4).
3.1.4. Classification into BrC Optical Classes. Figure 3
shows that the primary and aged African BB (organic-rich)
aerosols in the humid chamber are weakly to moderately
absorptive, which is typical of smoldering-dominated combus-
tion, and they are largely methanol-soluble (methanol extracts
accounted for 85−90% of total organic carbon mass; Text S2).
Classification into BrC optical classes49 is based on the short-
wavelength absorptivity (MAC405 nm) and its wavelength
dependence as expressed by the AAE.35 The AAE values of
3−7 at 370−470 nm fall within the range defined by previous
smoldering biomass combustion experiments (black rectan-
gles; AAEs at 405−532 nm), which included pine needles and
Siberian/Indonesian peat as well as featured in situ photo-
acoustic measurements with optical closure (see Siemens et
al.50 and references therein).
3.2. Quantification of BrC Aerosol Mass. The RPLC/
DAD-ESI-HR-QTOFMS/MS method (Section 2.4) effectively
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standards used for quantification (Table S2), 24 (40%) were

Figure 3. Optical absorption properties of primary and aged OAs (in
the humid chamber) derived from African biomass smoldering
combustion, plotted in the AAE − log10MAC405 space, building upon
Saleh49 and extended to shorter wavelengths by Hettiyadura et al.35
The AAE values were calculated over the wavelength range of 370−
470 nm for this study and from 350 nm up to 1000 nm in the
literature. Different BrC classes varying in absorptivity from very weak
(top left) to strong (bottom right) are represented by shaded areas.
Circles display the optical absorption properties of samples from this
study, derived from calibrated aethalometer measurements. Error bars
represent the uncertainty based on four repeated chamber experi-
ments (including different fuel types and all aging conditions) and the
aethalometer calibration uncertainty combined in quadrature.
Literature values from BB smoldering burns50 are represented by
squares, and the star symbols correspond to individual “tar-ball
particles” as inferred from electron energy loss spectro-micros-
copy.52,53
identified the majority of RPLC-separated BrC species in
ambient samples and the chamber-aerosol samples derived
from smoldering-dominated combustion, including BrC stand-
ards (Figures S2 and S3 and Table S2). Of the 60 BrC
ionized in both (−)ESI and (+)ESI, 18 (30%) were exclusive
to (−)ESI (including nitroaromatic compounds, NACs), and
18 (30%) were ionized solely in (+)ESI. ESI ionization
efficiency varies substantially between compounds due to their
distinct sizes and functional groups.51
We divided the RF of each BrC standard by the population
geometric mean per ion mode to obtain relative response
factors (RRFs; Figure S4). The 2 orders-of-magnitude
variability in RRFs underlines the necessity of using multiple
standards spanning a wide range of chemical classes,
structures/polarities, molecular weights, and retention times
to effectively quantify BrC species.
Figure 4 shows recovery-corrected mass contributions of 182
identified BrC species (Text S3, S4 and Table S4), determined
using the RFs of the 60 standard compounds (Table S2),
grouped into chemical classes. Shown are results from the
ambient-aerosol samples from Botswana, primary aerosol
emissions from all fuel types in the humid chamber, selected
dry chamber dark, and selected photochemically aged chamber
samples; chamber-aerosol samples were selected based on the
aethalometer data and trends (Figure 2 and Text S3). While
only 25% of the total identified BrC species had a matching
authentic standard, these species accounted for the majority of
the total identified BrC aerosol mass (mass fraction Q1−Q3
among samples: 0.52−0.64; Q: quartile).
3.2.1. Linking BrC Aerosol Mass to OA Absorption. A
strong linear relationship (Pearson’s r: 0.85) exists between the
fraction of the (OA-rich) PM that is BrC (i.e., the sum of
identified BrC species mass) and the MAC at the near-UV
wavelength. The linear-fit (Figure S5a) slope of 0.14 ± 0.02 m2
per g of total quantified BrC directly links BrC aerosol mass to
aerosol light-absorption cross section and, thus, can be used to
parametrize BrC in models. The correlation remains robust

Figure 4. Mass closure of all 182 BrC species identified through RPLC/DAD-ESI-HR-QTOFMS/MS using the RFs from Table S2 (RRFs shown
in Figure S4): (a) percentage contribution of different BrC chemical classes to the total quantified RPLC/ESI-HR-QTOFMS/MS-based BrC mass
in chamber- and ambient-aerosol filter samples, displayed as cumulative contributions, and (b) percentage contributions (cumulative) of each
chemical class to PM mass across samples�the highlighted lower subpanel corresponds to a distinct scale. The fuel mixture contained equal masses
of all fuels, excluding cow dung, to mimic a wildfire scenario with numerous biomass types. Refer to Figure S5 for the relationship between Figure
4b and OA absorptivity (Figure 1) and Figure S7 for the clustering of samples/compounds based on individual BrC species’ fractional
contributions to BrC mass.

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Figure 5. Molecular-level characteristics of all 182 identified BrC species that are shown in Table S4 (i.e., DAD-absorbing formulas identified with
ESI), including authentic standards (Table S2). These are categorized by chemical class (lignin pyrolysis products include substituted guaiacols/
syringols among other substituted benzenes) and display: DBE [DBE = C − (H/2) + (N/2) + 1] as a function of (a) measured (neutral) mass or
(b) carbon plus nitrogen atoms, (c) van Krevelen diagram displaying atomic O/C vs H/C ratios, and (d) average oxidation state of carbon [OSC =
(2 × O−H + 3 × N)/C] as a function of carbon-atom count. Note that some data points from the same or different chemical classes overlap. Panel
(b) demonstrates that all RPLC/DAD-ESI-HR-QTOFMS/MS-based absorbing formulas fall within the BrC-relevant space,30,50 with DBE/(C +
N) ratios ranging from 0.5 to 0.9, as indicated by the dashed lines.

(Pearson’s r: 0.89) even when only the mass of the BrC species
with matching authentic standards (∼60% of total quantified
BrC mass; Section 3.2) is considered for the x-axis values,
suggesting that the quantification approach with surrogate
standards does not influence the results. However, a perfect
linear relationship is generally not expected, as individual
chromophoric species with distinct MAC spectra contribute
variably to BrC/aerosol mass across samples. The effect of
sample-to-sample variability in chemical composition on this
relationship is highlighted by the higher linear-fit slope at 470
nm (Figure S5b) for photochemically aged BB emissions (0.10
± 0.03; Pearson’s r: 0.78) as compared to primary (dark-
chamber) and dark-aged emissions (0.03 ± 0.01; Pearson’s r:
0.81). This difference is attributed to the formation of visible-
light-absorbing NACs (Figure S3) upon irradiation of the
primary/dark-chamber emissions (Section 3.2.2 and Figure
2b).54
3.2.2. Mass Closure of Identified BrC Species Grouped into
Chemical Classes. While lignin pyrolysis products are
considered major contributors to BrC aerosols due to the
prevalence of lignin in biomass, their contribution to BrC mass
and variations due to photochemical aging have not previously
been characterized, to our knowledge.55 Figure 4a shows that
in the humid-chamber BB aerosol samples, the Q1−Q3
fractional contributions (first and third quartiles) to total
BrC mass (identified through RPLC/DAD-ESI-HR-
QTOFMS/MS; Section 2.4) by combined substituted
guaiacols, substituted syringols, and other substituted benzenes
(i.e., lignin pyrolysis products) as well as coumarins and
(stilbenes + flavonoids) are 0.08−0.15, 0.10−0.23, 0.45−0.62,
0.04−0.11, and 0.04−0.08, respectively. While lignin pyrolysis
products dominate the chamber BrC aerosol mass, NACs
F https://doi.org/10.1021/acs.est.3c09378
contribute significantly to photochemically aged BrC aerosols,
accounting for up to 12% in hardwood-derived BB emissions
and 30−60% for dung and leaves. In the ambient Botswana
PM samples, “other substituted benzenes” are the most
abundant among potential lignin pyrolysis products, whereas
higher molecular-weight BrC species (mainly coumarins and
flavonoids) collectively contribute up to 20% of BrC mass,
similar to chamber aerosols. NACs contribute up to 8 and 23%
of BrC mass in daytime and nighttime BIUST samples,
respectively, and 22−26% in Gaborone samples. Daytime−
nighttime sample comparisons suggest that ambient NACs
might form in the dark, prompting further research into the
simulated nighttime processing of African-BB primary BrC
emissions (e.g., with nitrate radicals,56 or in clouds/wet
aerosols57) and their daytime evolution.
Figure 4b shows that primary/dark-generated BrC aerosols
from the smoldering combustion of African hardwoods (acacia,
eucalyptus, mopane, mosetlha, mukusi, wanza, and wild olive)
in the humid chamber typically exhibit a higher relative
abundance in fine PM mass (OA-rich; 2.0−14%) as compared
to emissions from the combustion of cow dung, mokala
branches, mopane leaves, and savanna grass (0.4−3.6%).
Similar to MAC (Figure 2 and Section 3.1.3), this abundance is
influenced by chamber RH and UV exposure. Primary BB
emissions in the dry chamber contain 1.5 to 4.5 times more
BrC (in % of PM mass) compared to emissions from replicated
experiments in the humid chamber. On the other hand,
photochemical aging of primary emissions in the humid
chamber generally reduces the relative abundance of BrC by up
to 60%, except for leaves and dung where the formation of
NACs compensates for other BrC species losses (Figure 4b).
Section 4 further discusses these trends.
Environ. Sci. Technol. XXXX, XXX, XXX−XXX
Environmental Science & Technology
The relatively lower abundance of combined BrC species in
ambient PM (up to 0.2%) might be linked to a range of factors,
including a lower relative abundance of OA in PM compared
to chamber samples (which affects gas-to-particle partitioning
of semivolatile organics); BrC whitening due to complex aging
mechanisms in the atmosphere (e.g., photobleaching and
dilution-driven evaporation; Text S2); influence of other fuel
types or sources with lower BrC content (Text S2), such as
hydrocarbon-like (nonaromatic) emissions; high combustion
efficiency; lower solubility of ambient BrC in methanol
compared to chamber emissions; and the presence of coarse-
mode aerosol species (e.g., dust).
3.2.3. BrC vs PM EFs. The PM EF (EFPM; Text S2) for
smoldering combustion from African BB in the humid
chamber is 20 ± 5 g per kg of fuel burned, consistent with
our previous findings38 and largely independent of fuel type
(Table S1). This range is similar to reported values for
Western US wildfires (26 g PM1 kg−1)58 and smoldering
savanna and grassland fire smoke (∼10−25 g PM1 kg−1),6 as
well as traditional Tibetan biomass stoves (25 g kg−1) and
Ugandan 3-stone fires (15 g kg−1),59 but higher than South
Asian biomass stoves (7 g kg−1).59 In contrast, combined BrC
species EFs derived from African fuels in the humid chamber
show greater variability and depend on the fuel type, ranging
from <0.15 g BrC per kg for cow dung and mopane leaves to
∼1.7 g kg−1 for mukusi (Table S1). Sun et al. reported a
geometric mean EFBrC of 0.7 g kg−1 for Chinese household
biomass fuels (straw, stalk, pine, and pellets) under mixed-
combustion conditions.60
Figure S6 shows that the major humid-chamber primary BrC
aerosol species with a matching authentic standard are
sinapaldehyde (#86, Table S2), 1-phenyl-1,3-butanedione
(#64, Table S2), and nodakenetin (#102, Table S2), with
EFs up to ∼200 mg kg−1. These are followed, in descending
order of the 11-fuel mean EF, by 3-hydroxybenzoic acid (#35),
syringic acid (#46), coniferaldehyde (#85), acetosyringone
(#78), syringaldehyde (#69), 3,4-dihydroxybenzaldehyde
(#18), homovanillic acid (#47), pyrogallol (#3), 4-methyl-
catechol (#61), scopoletin (#73), vanillic acid (#36), and
vanillin (#60). Note that species-specific EFs are given by the
mass fraction of each BrC species in the total filter-collected
primary aerosol mass (Text S4), multiplied by the EFPM.
Chemical structures, along with other major species quantified
with surrogates, correspond to the IDs shown in Table S2. The
wide range of lower-to-upper percentiles emphasizes the
substantial fuel-to-fuel variability in BrC species EFs, with
the lowest values generally reported for dung and leaves.
Studies are warranted to determine additional fuel-specific EFs,
particularly for individual BrC species.61
3.3. Detailed BrC Molecular-Level Composition.
Figure 5 illustrates molecular-level characteristics of all 182
identified BrC species (Table S4).29 The double bond
equivalent (DBE) represents the total number of rings and π
bonds and increases from 4 to 6 for lignin pyrolysis products to
∼7−8, 9, and 10−12 for coumarins, stilbenes, and flavonoids,
respectively (Figure 5a). All identified chromophoric species
fall within the “BrC-relevant space”,30,50 characterized by
DBE/(C + N) ratios of 0.5−0.9 (Figure 5b). This indicates
some degree of conjugation across their molecular struc-
tures,30,50 which seems to be a crucial requirement for light
absorption. The van Krevelen plot (Figure 5c) and carbon
oxidation state (Figure 5d) indicate moderate oxygenation and
functionalization of the identified BrC species, consistent with
G https://doi.org/10.1021/acs.est.3c09378
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primary and moderately aged BB-OAs.62,63 The species-mass-
weighted atomic ratios (O/C, H/C) of the BrC aerosol
population in (humid/dry) chamber dark/primary, (humid/
dry) chamber photochemically aged, and ambient filter
samples are (0.35 ± 0.01, 0.99 ± 0.04), (0.44 ± 0.04, 0.94
± 0.07), and (0.46 ± 0.03, 0.88 ± 0.08), respectively (±
indicates the 1σ variability between samples).
We employed hierarchical clustering (Section 2.6 and Text
S6) to simplify the complex BrC molecular-level composition
matrix. Through this clustering (see dendrogram in Figure S7),
we discerned several distinct feature types and compared them
with those found in ambient PM samples. BrC species
introduced below for the first time will be specified by their
formula and ID from Table S4, and tentative structures
quantified using surrogate standards will be shown in italics.
Primary BrC aerosol species from burning savanna grass,
leaves, and cow dung are discussed in Text S7 as these samples
were less absorptive than hardwood-derived emissions (Figure
1).
3.3.1. Hardwood-Derived Primary BrC Species. In
chamber-aerosol samples, coniferaldehyde (C10H10O3, #85)
and sinapaldehyde (C11H12O4, #86) are major chromophoric
species, contributing ∼0.6% and 0.8−1.2%, respectively, of the
primary PM mass from wanza and mopane combustion in the
dry chamber. The coniferaldehyde/sinapaldehyde (C/S) mass
ratio in primary smoldering combustion emissions has a Q1−
Q3 range of 0.18−0.43. Photochemical aging in the humid
chamber reduces their abundance by 80−90% (in line with
Fleming et al.48) and 95%, respectively; the C/S mass ratio
increases >2.0 in nonhardwood-derived photochemically aged
emissions.
Hardwood-derived emissions exhibit up to 0.6, 0.1, and 0.1%
contribution to fine PM mass from vanillic acid (C8H8O4,
#36), its likely structural/positional isomer (RT = 12.4 min,
#31), and hydroxybenzoic acids (C7H6O3, #21 and #35),
respectively. All chamber aerosols, except for those from cow-
dung/leaf burning, contain syringic acid (C9H10O5, #46),
which contributes a maximum of 0.4% to PM mass. The most
abundant coumarin and substituted benzene detected in our
study are nodakenetin (C14H14O4, #102) and 1-phenyl-1,3-
butanedione (C10H10O2, #64), respectively. They represent
0.6−1.2 and 0.8−1.8%, respectively, of PM mass in primary BB
emissions from mukusi, acacia, wanza, and mopane. Both
compounds are highly sensitive, with 70% of nodakenetin lost
upon photochemical aging (corroborating Fleming et al.48); 1-
phenyl-1,3-butanedione vanished upon irradiation, likely due
to a photochemical reaction that occurs when the molecule
absorbs light energy, causing the bond adjacent to the carbonyl
group to break (Norrish type I cleavage64).
Furthermore, acetosyringone (C10H12O4, #78) is present in
all chamber-aerosol samples, contributing up to 0.3% to PM
mass. Catechol−resorcinol isomers (C6H6O2, #5 and #11) and
3,4-dihydroxybenzaldehyde (C7H6O3, #18) are more abundant
in primary emissions from mopane, mukusi, and wanza
combustion, particularly in the dry chamber, making up 0.6−
1 and 0.2% of PM mass. Homovanillic acid (C9H10O4, #47)
contributes 0.05−0.2% to PM in hardwood-derived primary
emissions. However, homovanillic acid and its likely positional
isomer (RT = 14.8 min, #50) are susceptible to photochemical
aging. Primary emissions of cinnamic acid (C9H8O2, #55) and
methoxycinnamic acid (C10H10O3, #70) are strongly correlated
with homovanillic acid, but the latter is 3 times less abundant.
Dihydroxy-cinnamic acid (C9H8O4, #51) is present in primary
Environ. Sci. Technol. XXXX, XXX, XXX−XXX
Environmental Science & Technology
BB aerosol emissions from mopane, wanza, and grass in the dry
chamber; however, its relative abundance decreases by 60−
90% in the humid chamber. Hydroxy-dimethoxychalcone
(C17H16O4, #172) contributes ∼0.05−0.1% to PM mass in
mopane-, mukusi-, and wanza-derived primary BrC aerosols.
3.3.2. Tracer BrC Species for African Hardwoods. We
identified several primary BrC species that serve as tracers for
specific hardwood species (Figure S7) within the range of
African biomass fuels included in this study. Pyrogallol
(C6H6O3, #3) serves as a tracer for primary emissions from
wanza combustion in the dry (1.9% of PM mass) or humid
chamber (0.7% of PM mass). Scopoletin (C10H8O4, #73), a
methoxy-hydroxycoumarin, is a tracer for primary emissions
from wild olive smoldering combustion (0.3% of PM mass),
along with hydroxytyrosol (C8H10O3, #10; 0.5% of PM mass),
tyrosol (C 8 H 10 O 2 , #24), esculetin (C 9 H 6 O 4 , #38),
(hydroxy-)dimethoxycoumarin isomers (C11H10O4−5, #79 and
#96), and hydroxy-methoxychalcone (C16H14O3, #118). How-
ever, we found that scopoletin is prone to photochemical aging
and could not detect it in ambient PM samples from Botswana.
On the other hand, dihydroxy-dimethoxyf lavone (C17H14O6,
#154), previously identified as a potential tracer for ceanothus
burning,48 is only detected in ambient PM samples from
BIUST and Gaborone. Another species native to Africa, not
among those in the literature study, must be producing
dihydroxy-dimethoxyflavone upon combustion since ceanothus
has a North American range. Hydroxy-trimethoxychalcone
isomers (C18H18O5, nos. 170 and #176) act as tracers for
wanza, mopane, and mukusi primary emissions. Coniferyl
ferulate or tetrahydroxyf lavanone (C20H20O6, #147) and
hexamethoxyflavone (C21H22O8, #150) contribute to primary
BrC aerosols emitted from burning mosetlha and eucalyptus,
respectively.
3.3.3. Evolution upon Simulated Photochemical Aging.
The formation of NACs is observed during photochemical
aging in the humid chamber, potentially mediated by HONO
that has been photolyzed by UV light. Abundant NACs, listed
in the order of increasing RT, include 4-nitrocatechol (#66) as
well as its positional isomers (#8; C6H5NO4), 5-nitrosalicylic
acid (C7H5NO5, #80), 4-nitrophenol (#87) as well as its
positional isomers (C6H5NO3, #2 and #12),
methoxy-nitrocatechol (C7H7NO5, #91), methoxy-nitrophenols
and methyl-nitrocatechols (#19, #92, and #100) such as 4-
nitroguaiacol (#95) and 2-methyl-4-nitroresorcinol
(C7H7NO4, #123), dimethoxy-nitrophenol (C8H9NO5, e.g.,
nitrosyringol, #99), dimethyl-nitrobenzoic acids (C9H9NO4,
#106, #116, and #120), nitroacetophenone or methyl-nitro-
benzaldehyde (C8H7NO3, #110), methyl-nitrophenols (#42 and
#44) including 4-nitro-o-cresol (C7H7NO3, #117), dimethoxy-
nitrobenzene (C8H9NO4, #128), and 4-nitro-1-naphthol
(C10H7NO3, #145). The most abundant NAC is 4-nitro-
catechol, which may be a product of the OH-initiated reaction
of catechol, accounting for 0.3−0.4% of PM mass in
photochemically aged emissions from mukusi and wanza.
The detected NACs correspond with previous findings in
chamber/ambient aerosols or cloud-water samples associated
with BB or mixed-source urban emissions.28,29,65−69
Furthermore, syringaldehyde (C9H10O4, #69) contributes up
to 0.4% of PM mass in photochemically aged emissions from
mopane, mukusi, and wanza. Vanillin (C8H8O3, #60) forms
upon photochemical aging of mukusi and wanza primary BB
emissions in the humid chamber (∼0.6% of PM mass),
suggesting that it may be an oxidation product of lignin formed
H https://doi.org/10.1021/acs.est.3c09378
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from the breakdown of larger aromatic compounds present in
primary BB emissions.70 Methoxy-catechol (C7H8O3, #57)
forms upon photochemical aging of hardwood-derived BB
emissions. Coumarin-carboxylate (C10H5O4, #67) exhibits
similar behavior and also appears in photochemically aged
emissions from leaf burning. Finally, acetovanillone (C9H10O3,
#72) contributes ∼0.03% to PM mass in photochemically aged
emissions from mukusi and wanza.
3.3.4. BrC Species in Ambient Aerosols and Similarities to
Chamber Aerosols. While photochemically aged chamber-
aerosol samples cluster together (Figure S7), the composition
of aged BrC from leaf and cow-dung burning exhibits unique
features, placing them in the same subcluster with ambient-
aerosol filter samples (Figure S7). For instance, increased
levels of compounds like 4-nitrocatechol, 4-nitrophenol, 4-
nitro-o-cresol, methoxy-nitrocatechol, 4-nitroguaiacol and its
positional isomers, the flavonoid kaempferol (C15H10O6,
#125), and coumarin-carboxylate are found in both the ambient
aerosols and photochemically aged emissions from leaf
burning. On the other hand, methylcatechol (C7H8O2, #37),
benzoic (C7H6O2, #81) and phthalic (C8H6O4, #20) acids,
(di)hydroxy-benzaldehydes (#18, #21, and #43), and methoxy-
nitrocatechol are found in both the ambient aerosols and
photochemically aged emissions from cow-dung combustion.
Additional BrC species that are common between ambient-
and primary/aged chamber-aerosol samples include the
following: 4-nitro-1-naphthol, nitrosyringol, dimethoxy-nitro-
benzene or methoxy-methyl-nitrophenol, and methoxy-nitro-
phenols or hydroxy-methyl-nitrophenols, which are present in
photochemically aged chamber-aerosol samples; terephthalic
(C8H6O4, #25) and phthalic acids, which contribute up to
0.03% and 0.1% of PM mass, respectively, collected in BIUST
and Gaborone and show levels comparable to those in
photochemically aged chamber-aerosol samples from mukusi
and wanza; p-coumaric acid isomers (#28 and #41) that
contribute significantly to BrC from hardwood and grass
burning (Text S7); and methoxy/dihydroxybenzoic acids
(C7H6O4, #9 and #82), hydroxybenzoic acid or dihydrox-
ybenzaldehyde (#21), hydroxy-benzaldehyde (C7H6O2, #26),
vanillin, (methyl-)umbelliferone (C9H6O3, #71 and C10H8O3,
#88), 3,4-dimethoxybenzoic acid (C9H10O4, #76), dihydroxy-
f lavone (C15H10O4, #152), and dihydroxyf lavanone or a
stilbenoid (C15H12O4, #155). Other contributing species to
BrC mass in the ambient-aerosol samples include hydroxyph-
thalic acid (C8H6O5, #17), dihydroxy-dimethoxyf lavone, as well
as a phenanthrenoid, chalcone, or f lavanone (C15H12O4, #173).
4. ATMOSPHERIC IMPLICATIONS
The impact of African BB aerosols on regional climate and
intercontinental air mass transport is significant.71,72 Our
research offers a comprehensive quantification of optical
absorption and molecular characteristics of African BB-derived
aerosols and sheds light on the implications of their
atmospheric processing. By systematically analyzing biomass
fuels from this understudied region,73 we have advanced the
fundamental understanding of the atmospheric chemistry of
BrC aerosols.74 We quantified a large number (182) of highly
absorptive (in the near-UV region) methanol-extractable
organic compounds in chamber smoldering burns of African
biomass. This detailed molecular analysis highlights the key
role of light-absorbing moieties, present in trace concentrations
(Figures 4 and S7), in driving particle-phase OA absorptivity.
While individual BrC species contribute <1−2% of fine PM
Environ. Sci. Technol. XXXX, XXX, XXX−XXX
Environmental Science & Technology
mass, in combination, they account for over 10% of PM mass
in some African fuels examined during our laboratory studies.
Besides identifying major contributing compounds, their
classes, and their EFs, we have pinpointed specific BrC tracer
species that can distinguish between different African biomass
fuels, aiding in source apportionment studies. Moreover, our
source/aging experiments have practical implications for
interpreting ambient air measurements. Notably, the photo-
chemically aged BrC emissions from leaf and cow-dung
combustion exhibit molecular fingerprints similar to those
found in ambient PM collected from Botswana (Figure S7),
offering a direct link to real-world conditions.
Our findings suggest a complex role of the phase state and
photochemistry in influencing the BrC composition and OA
absorptivity. At ∼ 65% chamber RH, we observed a reduction
in the relative abundance of primary BrC mass in PM (Figure
4b), which in turn reduces the OA absorptivity at 370 nm
(Figure 2a). Yet, changes in the molecular-level BrC
composition with varying RH are likely not significant (Figure
S7), and the fractional contributions from different BrC
chemical classes remained consistent in different states (Figure
4a). At elevated RH, the water absorbed by particles may
reduce their viscosity, potentially promoting the diffusion of
water-soluble BrC species into the gas phase. Furthermore, the
presence of moisture on the chamber walls might cause a
higher tendency for species to adhere to the wall compared to
the dry chamber condition. The latter could lead to potential
selective losses of BrC aerosol species or gases75,76 to the
chamber walls, affecting the intensive optical absorption
characteristics of primary BB aerosols. With photochemical
aging, the OA MAC reduction at 370 nm and enhancement at
longer wavelengths (Figure 2b) relate to the photochemical
degradation of lignin pyrolysis products and concurrent
formation of visible-light-absorbing NACs (Figures 4 and S3).
Current air quality and climate models tend to under-
estimate the impacts of BrC due to limited data. Our findings
are crucial for representing BrC aerosols in atmospheric
models and parametrizing their optical properties (Section 3.1
and 3.2.1), toward simulating their radiative forcing with
greater accuracy. The detailed characterization of BrC species
from diverse biomass fuels aids source apportionment efforts in
Africa, where BB is a major aerosol source, and existing
emission inventories often rely on data from North American
and European contexts. We provide necessary data to update
these inventories,77 enabling more accurate environmental
impact assessments of African BB-derived BrC emissions. This
research can also guide the development of integrated climate
change mitigation and air quality management policies78,79 to
minimize the impact of BB on human health and climate,
particularly in sub-Saharan Africa.
■ ASSOCIATED CONTENT
Data Availability Statement
Raw data that support the findings of this study are available
from the corresponding authors upon reasonable request. Data
presented in figures80 are publicly available in Zenodo (DOI:
10.5281/zenodo.10601481).
*
sı Supporting Information
The Supporting Information is available free of charge at
https://pubs.acs.org/doi/10.1021/acs.est.3c09378.
Information on the African biomass fuels, chamber
experiments and measurements, filter sample collection,
I https://doi.org/10.1021/acs.est.3c09378
pubs.acs.org/est Article
sample preparation for BrC molecular analysis, BrC
species quantification approach (including standard
preparation and analysis and recovery analysis),
justification for and limitations of the molecular-level
analysis methodology, hierarchical clustering, and BrC
molecular-level composition in nonhardwood-derived
emissions; information on the chamber- and ambient-
aerosol samples that were used for analyzing the
molecular composition of BrC, authentic standards
used to quantify BrC species detected in aerosol filter
samples, fragmentation information for BrC standards,
and the 182 separated BrC species identified in
chamber- and ambient-aerosol filter samples; and
geographical distributions of African hardwood biomass
fuels, extracted wavelength chromatogram of aerosol
filter sample extracts, mass absorption coefficient spectra
of BrC standards and their RRFs, scatter plots of BrC
mass closure result and OA absorptivity, BrC species’
EFs in the humid chamber, and hierarchical clustering of
BrC species’ fractional contributions to BrC mass in 35
aerosol filter extracts (PDF)
■ AUTHOR INFORMATION
Corresponding Authors
Vaios Moschos − Department of Physics, College of Science
and Technology, North Carolina A&T State University,
Greensboro, North Carolina 27411, United States;
Department of Environmental Sciences and Engineering,
Gillings School of Global Public Health, The University of
North Carolina at Chapel Hill, Chapel Hill, North Carolina
27516, United States; orcid.org/0000-0002-6251-4117;
Email: moschosv@yahoo.com, vmoschos@ncat.edu
Solomon Bililign − Department of Physics, College of Science
and Technology, North Carolina A&T State University,
Greensboro, North Carolina 27411, United States;
Department of Applied Sciences and Technology, College of
Science and Technology, North Carolina A&T State
University, Greensboro, North Carolina 27411, United
States; Email: bililign@ncat.edu
Jason D. Surratt − Department of Environmental Sciences and
Engineering, Gillings School of Global Public Health, The
University of North Carolina at Chapel Hill, Chapel Hill,
North Carolina 27516, United States; Department of
Chemistry, College of Arts and Sciences, The University of
North Carolina at Chapel Hill, Chapel Hill, North Carolina
27599, United States; orcid.org/0000-0002-6833-1450;
Email: surratt@unc.edu
Authors
Cade Christensen − Department of Chemistry, College of Arts
and Sciences, The University of North Carolina at Chapel
Hill, Chapel Hill, North Carolina 27599, United States
Megan Mouton − Department of Applied Sciences and
Technology, College of Science and Technology, North
Carolina A&T State University, Greensboro, North Carolina
27411, United States
Marc N. Fiddler − Department of Chemistry, College of
Science and Technology, North Carolina A&T State
University, Greensboro, North Carolina 27411, United States
Tommaso Isolabella − Department of Physics, University of
Genoa, 16146 Genoa, Italy; National Institute of Nuclear
Physics (INFN), 16146 Genoa, Italy
Environ. Sci. Technol. XXXX, XXX, XXX−XXX
Environmental Science & Technology
Federico Mazzei − Department of Physics, University of
Genoa, 16146 Genoa, Italy
Dario Massabò − Department of Physics, University of Genoa,
16146 Genoa, Italy
Barbara J. Turpin − Department of Environmental Sciences
and Engineering, Gillings School of Global Public Health,
The University of North Carolina at Chapel Hill, Chapel
Hill, North Carolina 27516, United States; orcid.org/
0000-0003-4513-4187
Complete contact information is available at:
https://pubs.acs.org/10.1021/acs.est.3c09378
Author Contributions
V.M.: conceptualization, data curation, formal analysis, funding
acquisition, investigation, methodology, project administration,
validation, visualization, and writing�original draft; C.C.:
investigation and methodology; M.M.: investigation; M.N.F.:
conceptualization, funding acquisition, investigation, and
methodology; T.I.: formal analysis; F.M.: investigation; D.M.:
resources and validation; B.J.T.: conceptualization, funding
acquisition, and methodology; S.B.: conceptualization, funding
acquisition, resources, and supervision. J.D.S.: conceptualiza-
tion, funding acquisition, methodology, resources, and super-
vision. Review and editing: all coauthors.
Notes
The authors declare no competing financial interest.
▽ (8) Commission on Social Determinants of Health. Closing the Gap
Megan M. McRee was formerly known as Megan Mouton.
■ ACKNOWLEDGMENTS
This research was supported by the US National Science
Foundation (NSF) through the Atmospheric & Geospace
Sciences (AGS) Division grant # 2100708. V.M. acknowledges
support by the Swiss National Science Foundation (SNSF)
under the Postdoc.Mobility Fellowship grant
P500PN_210745. Field collection was funded by the NSF
Office of International Science & Engineering (OISE) Division
grant # 1559308. We thank Gizaw Mengistu Tsidu (BIUST)
for providing biomass fuel samples from Botswana and his
support during the BIUST field campaign and Christina Isaxon
(Lund University) for providing the cow-dung fuel sample
from Ethiopia. We also thank Janica Gordon (NC A&T) for
assistance with filter collections in Botswana and Naomi Chang
(UNC-Chapel Hill) for assistance with thermal-optical carbon
analysis.
■ ACRONYMS
AAE, absorption Ångströ m exponent; AEF, absorption
emission factor; AE33, aethalometer model 33; ATN,
attenuation; BB, biomass burning; BrC, brown carbon; DAD,
diode array detection; EF, emission factor (mass-based); ESI,
electrospray ionization; HR-QTOFMS/MS, high-resolution
quadrupole time-of-flight tandem mass spectrometry; MAC,
mass-absorption cross-section; MCE, modified combustion
efficiency; MWAA, multiwavelength absorption analyzer;
NACs, nitroaromatic compounds; OAs, organic aerosols;
PM, particulate matter; RH, relative humidity; RPLC,
reversed-phase liquid chromatography; (R)RF, (relative)
response factor; RT, retention time
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