Moteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12
https://doi.org/10.1186/s40645-023-00544-4

Progress in Earth andPlanetary Science

Open Access

REVIEW

Climate‑relevant properties of black carbon
aerosols revealed by in situ measurements:
a review
Nobuhiro Moteki1*   

Abstract
Light-absorbing aerosols affect atmospheric radiation, dynamics, and precipitations through shortwave absorption in
the atmosphere and snowpack. Black carbon (BC) is considered the most significant contributor to global shortwave
absorption among all the known light-absorbing aerosol components. In analyses and predictions of BC’s lifecycle
and climate effects, multiscale field observations are needed to test the fundamental assumptions in the climate
model. In situ measurements, the focus of this review, fill the gap of observational information accessible from remotesensing and laboratory analyses. This article reviews historical backgrounds, recent advances in in situ measurementsof BC, and the resulting observational findings used to update the assumptions in climate models and remote sensing. Finally, we raise open problems that demand a rethinking and future investigation.
Keywords Atmospheric chemistry, Atmospheric radiation, Climate, Aerosol, Light-absorbing aerosols, Black carbon
1 Introduction
1.1 Light‑absorbing aerosols

Light-absorbing aerosol components exert complex perturbations to the climate system through their shortwave
absorption in the atmosphere and snowpack (Stier et al.
2007; Samset et al. 2018). The atmospheric heating by
aerosol’s shortwave absorption alters the circulation andprecipitation from regional-to-global scales (Lau et al.
2006; Samset et al. 2022). Known significant contributors to aerosol’s shortwave absorption are light-absorbing constituents of carbonaceous compounds (i.e., black
carbon, brown carbon) and iron oxides (i.e., goethite,hematite, magnetite) from both anthropogenic and nonanthropogenic origins (e.g., Moteki et al. 2017).
Carbonaceous aerosol emitted as a byproduct of the
combustions of fossil fuels, biofuels, and biomass is a
*Correspondence:
Nobuhiro Moteki
moteki@eps.s.u-tokyo.ac.jp
1
Department of Earth and Planetary Science, Graduate School of Science,
The University of Tokyo, 7‑3‑1 Hongo, Bunkyo‑Ku, Tokyo 113‑0033, Japan

mixture of a large variety of organic molecules and partly
graphitized solid carbon (Lighty et al. 2000; Simoneit
2000). In addition, other organic molecules and polymers
as secondary constituents of carbonaceous aerosol are
produced in the atmosphere through gas-phase photochemical reactions and aqueous reactions in cloud droplets (Kalberer et al. 2004; Kanakidou et al. 2005; Ervens
et al. 2011; Shrivastava et al. 2017). Carbonaceous aerosol
materials can be categorized on the continuous spectrumof the imaginary part of the refractive index (Andreae
and Gelencsér 2006; Corbin et al. 2019). One extreme ofthe spectrum is the group of non-refractory organic molecules with negligible imaginary refractive index, whichis referred to as organic carbon (OC). Another spectrum extreme is the group of partly graphitized solidstate refractory material with a high imaginary refractive
index, black carbon (BC) (Bond et al. 2013). The middle of the spectrum is a group of yellowish-to-brownish
organic compounds with a moderate imaginary refractive index, commonly referred to as brown carbon (BrC)(Laskin et al. 2015). The BrC can also secondarily form
through photochemical reactions in the atmosphere© The Author(s) 2023, corrected publication 2023. Open Access This article is licensed under a Creative Commons Attribution 4.0
International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you
give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes
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view a copy of this licence, visit http://​creat​iveco​mmons.​org/​licen​ses/​by/4.​0/.

Moteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

from primary and secondary OC materials (Updyke et al.
2012). The imaginary refractive index of BrC material can
rapidly change as the BrC particles photochemically age
in the atmosphere (Zhao et al. 2015). By contrast, BC ischemically inert in the atmosphere and even persistentafter deposition on timescales from centuries to millennia (Coppola et al. 2022).
In this review, the author focused only on BC among all
the light-absorbing aerosol components to elaborate on
the recent advances in the in situ BC measurements andtheir contributions to the fundamental understanding ofaerosol processes and the developments of the aerosolclimate model.
1.2 Black carbon

Owing to its high imaginary refractive index and relatively long atmospheric lifetime, BC is the largest
contributor to global shortwave absorption in the present atmosphere among all the light-absorbing aerosol compounds (Samset et al. 2018; Sand et al. 2021).
Atmospheric heating by BC reduces the global mean precipitation by compensating for the latent-heat transport
from the surface to the atmosphere (Pendergrass andHartmann 2012). BC deposited on snow-covered surfaces contributes to albedo reduction and accelerates thesnowmelt (Flanner et al. 2007).
The morphology of each BC particle is known to be anaggregate of nanospheres. The diameter of each primarynanosphere (monomer) is typically 10–100 nm (Buseck
et al. 2014). Each monomer consists of an onion-shell-likearrangement of graphene nanolayers (Buseck et al. 2014).
The refractive index of each carbon monomer depends
on the electronic structure of the carbon material, whichis related to the degree of graphitization (Stagg andCharalampopoulos 1993; Bond and Bergstrom 2006). As
the degree of graphitization of BC particles depends onthe flame environment (Apicella et al. 2018), the refractive index of atmospheric BC could be variable depending on emission sources. The optical properties, such as
the mass absorption cross section (MAC ­m2/g), of eachBC particle depend on the refractive index of consisting
monomers, morphological parameters of aggregate, andaggregate’s volume-equivalent size relative to the wavelength (Zheng and Wu 2021).
Each BC particle emitted from the combusting flame
to the atmosphere rapidly undergoes internal mixing
with other aerosol components (e.g., organic matter,
sulfate, nitrate) through the condensation and coagulation process. Low-efficiency combustions such as wildfire produce high-concentration condensable organic
molecules and carbonaceous aerosols with a high OCto-BC ratio, resulting in instantaneous internal mixingof BC and OC within the dense smoke (Schwarz et al.

Page 2 of 16

2008b). By contrast, relatively high-efficiency combustions such as vehicle engines produce carbonaceous
aerosols with a much lower OC-to-BC ratio, resulting
in the release of uncoated pure BC particles into theatmosphere (Schwarz et al. 2008b). Such BC particles
undergo internal mixing with secondary aerosols (e.g.,organics, sulfate) formed through the photochemical
production of condensable gases from precursors (i.e.,
volatile organic compounds, sulfur dioxide, ammonia, etc.) (Shiraiwa et al. 2007; Riemer et al. 2010).
Two dominant aerosol components mixed with BC areconsidered to be sulfate and organics because of thepervasiveness of these compounds in the atmosphere(Murphy et al. 1998; Thompson et al. 2022).
The BC-containing particles consisting of BC andnon-BC materials are very different in climate-relevant
properties from pure BC particles. Firstly, BC-containing particles consisting of BC core and non-absorbing
coating materials have larger MAC per unit BC mass
than pure BC particles due to enhancement of theelectric field incident onto the BC core through “lensing effects” by the coating materials (Fuller et al. 1999).
The MAC enhancement of ambient BC by coating may
be up to ~ 60% depending on sources and aging (Liuet al. 2017). Secondly, BC-containing particles would
be able to be cloud condensation nuclei (CCN) undermodest supersaturations (~ 0.1%) in environmental
clouds, whereas the pure BC particles are CCN inactive for their hydrophobic surface (Dusek et al. 2006;
Kuwata et al. 2009). The coating materials on the BC
core tend to become more hygroscopic with the agingof the plume (Ohata et al. 2016; Perring et al. 2017).
The coating strongly affects the critical supersaturationof BC-containing particles in less-aged urban plumes(Zaveri et al. 2010). The thickness and hygroscopicityof the coating are, therefore, critical factors controllingthe efficiency of vertical transport of BC through moist
convection at the proximity of urban emission sources(Moteki et al. 2019).
In this review, we provide the historical backgrounds
and recent advances of the in situ techniques for identifying and quantifying the BC and BC-containing particles after the mid-2000s. We clarify the unique roles ofin situ BC measurements in recent advances in physicalscience basis on evaluating the effects of BC and otheraerosols on climate (Fig. 1). This review on BC is intentionally focused on the research areas the author (N.
Moteki) has made some original contributions, avoiding
the areas already reviewed by previous studies (e.g., Bondand Bergstrom 2006; Ramanathan and Carmichael 2008;
Moosmüller et al. 2009; Bond et al. 2013; Petzold et al.
2013; Kang et al. 2020; Liu et al. 2020a, b; Coppola et al.
2022).

Moteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

Page 3 of 16

Fig. 1 Roles and relationships of the four different approaches in aerosol-climate research. Laboratory analyses of collected samples, in situ
measurements, and remote sensing provide complementary observational information needed for reducing assumptions in the atmosphericchemical transport model (sub-module of the climate model)

2 Measurement techniques
2.1 Backgrounds

BC is a ubiquitous aerosol component from the troposphere to the stratosphere, but its abundance is only atiny fraction (< 2%) of total submicron aerosols mass in
the global atmosphere, most of which is contributed bysulfate and organics (Gao et al. 2022). The minority of BC
in the total aerosol carbon with various physicochemical
properties makes the robust thermochemical identification of BC difficult (Cavalli et al. 2010; Karanasiou et al.
2015). Bulk optical methods for quantifying BC according to the absorption spectrum of a population of aerosol
particles require the assumptions of the spectral refractive index of every potential contributor to the measured
light absorption (Yang et al. 2009; Schuster et al. 2016).
In addition to the uncertainties of the spectral refractive
index, the change of light absorption efficiency of eachabsorbing component with particle’s size, morphology,
and mixing state with non-absorbing compounds makes
the bulk optical methods more susceptible to bias (Bondet al. 1999; Nakayama et al. 2010; Moteki et al. 2010a).
An observable particle-size measure of each BC aggregate depends on the measurement principle and procedure due to the non-spherical particle shape and internal
mixing with other components (Kasper 1982; McMurry
et al. 2002; Slowik et al. 2004; Kazemimanesh et al. 2022).
BC aggregates change their original lacy shape to be morecompact in the atmosphere as they experience collapsing
through their aging and cloud processing (Bhandari et al.
2019). For these reasons, it has been difficult to quantify
the size-resolved BC concentration with a size-sorting
aerosol sampling followed by bulk BC analyses.
The single-particle laser-induced incandescence (LII)
using an intracavity laser beam introduced around the
mid-2000s (Stephens et al. 2003), a commercial version is known as single-particle soot photometer (SP2;
Droplet Measurement Technologies Inc., Boulder, CO.),has extended our capability of identifying and quantifying atmospheric BC and BC-containing particles largely
overcoming the difficulties mentioned above. The in situ
data obtained by the SP2 instruments are routinely usedin the aerosol-climate research community for investigating aerosol processes and testing and prescribing
assumptions in other BC monitoring methods, aerosol
remote sensing algorithms, and aerosol-climate models. We review the development history, principle, andknown limitations of the single-particle LII in Sect. 2.2.
We would use the word single-particle LII instead of SP2
as we focus here on the physical principle, independentof the supplier’s actual implementation of the hardware
and software.
Section 2.3 reviews complex amplitude sensing (CAS)(Moteki 2021), a generic method for single-particle optical characterization of liquid-borne particles, which isMoteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

also useful as a new approach for in situ BC measurements and explorations of BC refractive index.
2.2 Laser‑induced incandescence

The laser-induced incandescence (LII) using pulsed lasers
has long been used in combustion sciences for the noninvasive characterization of concentrations and microphysical properties of soot particles in flame (Vander Wal andWeiland 1994; Schulz et al. 2006; Michelsen et al. 2015).
In the pulse LII approach, each high-energy pulse of alaser beam emitted from the light source (e.g., Nd:YAG
laser) is expanded to irradiate a flaming volume that contains a population of soot particles. Then, the thermalradiation at visible-to-near-infrared wavelengths, also
called incandescence, emitted from soot particles heated
up to their vaporization point ~ 4200 K, is detected atseveral wavelength bands by photodetectors or image
sensors. The simultaneous LII measurement at several(at least two) wavelength bands is needed for estimating the soot temperature from the spectral dependenceof emitted thermal radiation. LII signal intensity at eachwavelength band is proportional to the soot volume concentration within the sensing region. Imaging LII intensity distributions resolves the soot-forming regions andsoot population growth within the flame (Ni et al. 1995).
The rate of cooling of soot particles after the excitation
pulse inferred from a fast time-resolved measurement of
LII signals is used to estimate the mean monomer size ofsoot aggregates (Vander Wal et al. 1999; Axelsson et al.
2000). The pulse energy density for LII excitation within
the sensing volume is determined between the lower
limit that is needed to heat soot particles to vaporization point and the upper limit at which vaporization lossof soot during the pulse excitation starts to be apparent(Vander Wal and Jensen 1998). The laser wavelength for
LII excitation should be selected to reduce the interferences from fluorescence emission of clusters of carbon
atoms (Goulay et al. 2009). The longer excitation wavelengths are preferable to suppress fluorescence at the LII
monitoring visible wavelengths, whereas the particle’s
heating efficiency is higher in shorter excitation wavelengths (Schulz et al. 2006). The near-infrared 1064 nm
wavelength of Nd:YAG laser or its second harmonic
532 nm was primarily employed for LII excitation inpractice (Michelsen et al. 2015).
Although the pulse LII approach is used for monitoring the volume concentration of BC particles in engine
exhaust gases (Snelling et al. 1999), it is not practical forfield observations due to the very low and highly variable
BC concentrations in the atmosphere. Pulse-hit probability can be increased if the excitation pulse is triggered by
the particle’s scattering signal from another continuous
wave (CW)-operating laser beam just upstream of the LIIPage 4 of 16

excitation region, as has been done in the single-particle
laser mass spectrometers (Murphy 2007). Even so, BC
detection frequency in ambient air samples will remain
too low to obtain size-resolved statistics in real-time as
the fraction of aerosol particles containing BC aggregate
will be one-to-several orders of magnitude lower thanBC-free particles (Matsui et al. 2011).
The particle detection frequency drawback of pulse LII
for atmospheric applications has been concisely solvedby the single-particle LII technique using an intracavity
CW-laser beam (Stephens et al. 2003). The single-particle
LII uses the CW-laser beam building up inside a solidstate laser cavity to excite the LII signal from every BC(and other metallic) particle in the sample gas jet focused
into the intracavity beam. The original single-particle
LII instrument by Stephens et al. (2003) employed the1064 nm Nd:YAG laser cavity pumped by an 808 nm
fiber-coupled diode laser (< ~ 4W). This diode-pumped
Nd:YAG 1064 nm laser system has been employed bymost of the single-particle LII instruments developed so
far for its practical energy efficiency, stability, and costadvantages. The original instrument by Stephens et al.
(2003) integrated four independent light-collection optics
with different optical filters to be able to simultaneously
monitor four different signals from each particle during
its transition across the intracavity beam: three of whichwere used for LII signals at various wavelength bands,
one of which was used for scattering signal at 1064 wavelength. The waveform of the scattering signal was initiallyused as an indicator of the particle’s vaporization in thelaser beam. An appreciable shrink of an incandescing
particle in the laser beam is experimental evidence thatthe particle’s temperature has reached the material-specific vaporization point at the peak of LII signals. The signal intensity ratios between the three LII channels wereused for identifying incandescing material according to
the difference in vaporization temperature. Although
Stephens et al. (2003) demonstrated single-particle LII’s
capability to identify individual flame soot, graphite, andseveral metallic particles, they did not investigate thepossibility of quantifying the climate-relevant propertiesof single BC particles (e.g., size, mixing state).
Baumgardner et al. (2004) reported the first applicationof a single-particle LII instrument (single-particle sootphotometer: SP2 commercialized by Droplet Measurement Technologies) to field observations. Determining
single-particle BC mass from the LII signal in field observations requires a laboratory calibration of their empirical relationship using an appropriate standard BC sample.
Baumgardner et al. (2004) used a spherical glassy carbon
powder to sort particle mass using a conventional electrical mobility particle-size classifier (Knutson and Whitby
1975). The potential artifacts of using the spherical glassy

Moteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

carbon as an LII calibration standard material for quantifying non-spherical BC aggregates were not evaluatedthen.
Schwarz et al. (2006) and Slowik et al. (2007) employed
flame-generated soot as more similar materials with
ambient BC aggregates for calibrating the LII-to-mass
relationship within 2–30 fg mass range (130–320 nm
volume-equivalent diameter dv, assuming 1.8 g ­cm−3
density). In the calibration, they indirectly estimated themass of flame-generated soot particles sorted at a particular mobility diameter by scanning their distribution
in vacuum aerodynamic diameter, as a direct method forsorting the mass of non-spherical aerosol particles had
not yet been available. Schwarz et al. (2006) observedthat the LII signal amplitude was linearly proportional tothe mass of flame-generated soot at 2–30 fg and that thelinear relationship (e.g., slope) was unchanged with thefractal dimension of soot aggregates. They employed thelinear LII-to-mass relationship for ambient BC measurements, extrapolating the calibration line at mass ≤ 30 fg
to larger particles up to ~ 800 fg (dv ~ 950 nm). Although
the accuracy of this extrapolation had not been thoroughly evaluated then, Schwarz et al. (2006) are regarded
as a pioneering work providing quantitative altitude profiles of ambient BC concentration from the troposphereto the lower stratosphere for the first time by using awell-characterized single-particle LII instrument.
Moteki and Kondo (2007) have experimentally shownthat even thick coating on the BC core by low-volatility
organic materials (glycerol and oleic acid) does not affectthe single-particle LII signals from the BC core. They also
provided physical interpretations of the observed LII andscattering signal waveforms of BC-containing particles
using a numerical model simulating the time-dependent
particle’s properties in an intracavity laser beam.
Gao et al. (2007) developed a novel method to directly
measure the time-dependent position of the particle
translating across an intracavity Gaussian laser beam byusing a position-sensitive multi-element scattering detector placed at one of the four optical detection channels in
the SP2 instrument. The scattering signal waveform fromthe position-sensitive detector enables a reconstruction of the scattering amplitude of each particle before
evaporation. The coating thickness on the BC core canbe theoretically estimated from the scattering amplitudeof the BC-containing particle before evaporation. Moteki
and Kondo (2008) developed another method to estimate
the time-dependent position of each scattering particle
translating across a Gaussian laser beam from the normalized derivative of the scattering signal waveform.
This method enables a single-particle quantification of
coating thickness on the BC core without installing a
multi-element photodetector instead of a single-element

Page 5 of 16

photodetector. Although the random measurement error
in Moteki and Kondo (2008)’s method is more susceptible
to background noise in scattering signal waveform thanGao et al. (2007)’s method, the former will also be practically advantageous as it enables a reconstruction of thetime-dependent scattering cross section of BC-containing particle using only a signal waveform from a single
light-scattering photodetector. Later, the time-dependent
scattering cross section of each incandescing particle wasfound to help identify the morphological type (attachedor coated type) of BC-containing particles (Moteki et al.
2014) as well as for categorizing incandescing iron oxide
particles either of anthropogenic or desert dust origin(Moteki et al. 2017).
Moteki and Kondo (2010) characterized the LII-tomass relationships for various BC samples using a newly
available device for sorting the mass of aerosol particles
accurately according to the balance between centrifugal and electrostatic forces acting on the aerosols (aerosol particle mass analyzer (APM); Ehara et al. 1996).
APM enabled for the first time a sorting of aerosols bymass without particle shape-dependent bias and allowed
the accurate calibration of single-particle LII instruments using non-spherical BC particles. Moteki andKondo (2010) showed that the LII-to-mass relationshipdepends on both particle’s refractive index and shape.
The observed dependences were physically interpretable by the generalized Kirchhoff ’s law (Rytov 1953), as
experimentally confirmed by Moteki et al. (2009) and
Moteki et al. (2011). The linear proportionality between
LII signal amplitude and BC mass, frequently assumed
in SP2-related publications, is satisfied only if the radiation at the wavelengths used for incandescence detection(typically within 300–750 nm) can penetrate the entire
volume of a BC particle if the radiation counterpropagating from the observation point incident onto the BC
particle. This condition is satisfied when the size of BC
aggregate is smaller than the wavelengths. In larger particle-size domains, the LII-to-mass relationship becomes
nonlinear and strongly depends on the compactness ofparticle shape. Moteki and Kondo (2010) could not concretely demonstrate the dependence of the LII-to-masslinear slope to the BC refractive index at the smaller
particle-size domain because of the several theoreticalassumptions in their method for refractive index estimation (Moteki et al. 2010b). An experimental determination of the refractive index of BC at visible wavelengths
has been one of the open problems in aerosol-climate sciences, which will be discussed again in Sect. 3.
Because of the similarity in LII-to-mass linear slope
at the smaller size domain with ambient BC and diesel soot particles (Laborde et al. 2012) and the ease ofparticle generation, fullerene soot (Alfa Aesar Inc.) has

Moteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

been recommended as a standard BC powder material
for calibrating single-particle LII instruments (Baumgardner et al. 2012). At the larger particle-size domain(i.e., size >  ~ LII wavelength), nonlinearity due to theshape effects should be considered. This considerationis crucial in measurements of BC mass concentrationin rain and snow samples, wherein the BC size distributions tend to shift larger than in the atmosphere(e.g., Schwarz et al. 2013; Kinase et al. 2020; Mori et al.
2021).
The single-particle LII method is also able to detect
light-absorbing iron oxides from desert dust (Liu et al.
2018) and anthropogenic combustion sources (e.g.,
vehicles) (Moteki et al. 2017; Ohata et al. 2018). Laboratory experiments showed that the particle’s incandescence efficiency in a given operating laser powerof black-colored iron oxides (magnetite and wüstite)
is comparable to BC, whereas red-colored hematite showed lower efficiency. Notably, the LII-to-Femass relationship was observed to be identical among
wüstite, magnetite, and hematite (Yoshida et al. 2016;
Mori et al. 2023). In addition, the LII signal’s particlesize and spectral dependences agreed with the theoretical emission cross section according to Mie theory(Yoshida et al. 2018). These results suggest that eachsolid non-spherical particle consisting of any of wüstite(Fe(II)), magnetite (Fe(II, III)), and hematite (Fe(III))
has transformed into a molten iron (Fe) droplet in alaser beam before it starts to incandesce at boilingpoint (~ 3300 K). This fact allows theoretical extrapolation of the LII-to-Fe-mass relationship assuming spherical Fe particle beyond the upper particle mass limit
sortable using the APM, that is, ~ 1000 fg or ~ 700 nm
in volume-equivalent diameter (Yoshida et al. 2016;
Mori et al. 2023). This extrapolation is essential inatmospheric measurements as most of the anthropogenic iron oxide mass concentration is distributed
beyond ~ 700 nm volume-equivalent diameter (Moteki
et al. 2017; Yoshida et al. 2020).
After the above development efforts over two decades, the single-particle LII method, also known ascommercialized instrument SP2, has become a standard method for identifying and quantifying BC andBC-containing particles in the atmosphere essentiallywithout the limit of lowest detectable number concentration. The single-particle LII with a nebulizer has also
been the quantitative method for measuring BC in precipitated freshwater samples (e.g., rainwater, snowpack,ice sheets).
Corbin and Gysel-Beer et al. (2019) demonstrate thepossibility of identifying strongly light-absorbing spherical BrC particles (i.e., tarball; Pósfai et al. 2004) using thesingle-particle LII.

Page 6 of 16

2.3 Complex amplitude sensor

We briefly review another recent method for opticalparticle characterization, the complex amplitude sensor,
which is useful for in-line BC measurements. The complex scattering amplitude S = ReS + iImS =|S|ei∆ represents the amplitude |S| and phase shift ∆ of the scatteredfield relative to those of the plane-wave field incident
to the scattering particle (van de Hulst 1957). The S is afunction of the angle θ between the incident beam andobservation direction. The S reflects the physical properties of the scattering particle, such as refractive index,
volume, shape, and orientation, and thus plays pivotal
roles in optical particle characterizations and remotesensing of aerosols and clouds (Jones 1999; Romanovand Yurkin 2021). Light-scattering sensors, including
the optical particle counters, nephelometers, and remotesensing methods for reflected and scattered radiations,are designed to measure the power of the scattered field|S(θ)|2 at θ ≠ 0°, avoiding the direct optical beam of theincident field. On the other hand, light extinction sensors, including occultation single-particle sensors, cavityringdown extinction spectroscopies, and remote sensing
methods for direct radiation, are designed to measure theinterference power of the scattered and incident fields inthe forward direction ImS(0°) by monitoring the direct
beam (Mishchenko 2014). Simultaneous measurement ofboth ReS and ImS of suspended single particles has notbeen possible until recently because of its technical difficulties, as reviewed in Moteki (2021).
The self-reference interferometry of a forward-scattered field of single particles excited by a focused Gaussian beam, proposed by Giglio and Potenza (2011) anddemonstrated by Potenza et al. (2015), has been further refined by Moteki (2021) as a principle to be able
to measure the complex forward-scattering amplitude
S(0°) of single particles in liquid flow. We refer to it ascomplex amplitude sensor/sensing (CAS). The theoretical principle and hardware requirements for CAS havebeen described in Moteki (2021). The single-particle
S(0°)-measurements with CAS enable a rigorous optical characterization of single spherical non-absorbing
particles, which have only two unknown parameters(i.e., the real part of refractive index and diameter). The
single-particle S(0°)-measurements enable the identification and classification of different particle populations(e.g., black carbon, mineral dust, bacteria) coexisting inan environmental water sample, thanks to the sensitivityof the location of S(0°)-cluster to the difference in material properties (complex refractive index, shape) of thesize-distributed particle population (Yoshida et al. 2022).
Moteki (2020) proposed an algorithm to constrain eachparticle population’s complex refractive index, shape,and volume-equivalent size distribution from a distinct

Moteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

S(0°)-cluster. This algorithm has been further refined by
Moteki et al. (2023) and used to constrain the real andimaginary parts of the refractive index of ambient BC, as
to be detailed in Sect. 3.4.

3 Observational findings
3.1 BC in the global atmosphereBC mass concentration in the atmosphere had beennearly unknown before the single-particle LII (SP2 andits modified versions) became available for field observations. Here, we review the basic knowledge of atmospheric BC revealed from the single-particle LII. BC
mass mixing ratio in the midlatitude continental atmosphere shows a steep vertical gradient in the lower troposphere, decreasing from ~ 100 ng (kg air)−1 near thesurface to ~ 1 − 10 ng (kg air)−1 in the middle troposphere(Schwarz et al. 2006). BC mass mixing ratio level could
be ~ 10 times larger than this profile in the regions aroundlarge emission sources (e.g., East Asia) (Oshima et al.
2012; Kondo et al. 2016). BC mass mixing ratio in the
remote Pacific ocean was within the range of ~ 0.1 − 10 ng(kg air)−1 with a weak vertical gradient in the lower-toupper troposphere (Schwarz et al. 2010; Katich et al.
2018). BC mass mixing ratio over the remote Atlantic
Ocean tends to be substantially higher than the Pacific
Ocean due to the proximity to continental sources in
midlatitudes and the strong influence of African biomassburning in tropical latitudes (Katich et al. 2018). The BC
mass fraction was ~ 1–2% or less of the total submicronaerosol mass (Schwarz et al. 2006; Gao et al. 2022). BC
mass mixing ratio in the tropical tropopause layer, which
is a gateway of injection of tropospheric aerosols into
the stratosphere, was found to be ~ 1 ng (kg air)−1 (Gaoet al. 2008), which was similar to the average value in theupper troposphere to lower stratosphere over the midlatitude (Schwarz et al. 2006). The global atmospheric BC
data from the surface to upper troposphere are essential
to evaluate the model assumptions on the emission andtransport processes, as the new atmospheric BC dataset
had revealed the model bias of a factor of ~ 10 or morein remote regions and higher altitudes (e.g., Koch et al.
2009; Wang et al. 2014; Katich et al. 2018). The observational datasets of BC mass mixing ratio in the global
troposphere play critical roles in testing the assumptions of the parameters controlling the BC lifetime (e.g.,
the timescale of hydrophobic to hygroscopic conversion,
in-cloud scavenging efficiency) in global models (Kipling
et al. 2013; Hodnebrog et al. 2014; Lund et al. 2018; Liuand Matsui 2021).
Particle-size distribution of BC mass mixing ratio is
approximated well with a log-normal distribution withthe mode at ~ 200 ± 50 nm volume-equivalent BC core
diameter, being reasonably independent of location andPage 7 of 16

altitude up to the lower stratosphere (Schwarz et al.
2008a, 2010; Spackman et al. 2010; Kondo et al. 2011a;
Laborde et al. 2013; Reddington et al. 2013; Schulz et al.
2019; Yang et al. 2019; Yoshida et al. 2020; Ohata et al.
2021b). Even though fresh urban plumes could exhibit
smaller BC core size distribution <  ~ 150 nm (Schwarz
et al. 2008a; Laborde et al. 2013), the smaller distribution near the urban area will be of minor significancein regional-to-global scale as it transforms via coagulations to the stable distribution with the mode at ~ 200 nm
in ~ 1 day after emission (Moteki et al. 2007; Miyakawa
et al. 2017). Simultaneous observations of BC core size
distribution in the atmosphere and rainwater provided
observational evidence of the predominance of nucleation scavenging as a process controlling the efficiency of
wet removal of submicron aerosols (Ohata et al. 2016;
Moteki et al. 2019). Preferential removal of larger aerosol particles (with less critical supersaturation) throughmoist convections tends to shift the BC size distribution
to smaller in cleaner, particle-free air masses (Moteki
et al. 2012; Taylor et al. 2014; Schulz et al. 2019). The two
opposite size-regulating processes control the size distribution of BC in the atmosphere: the coagulation growthin the dense plumes just after emission and the preferential removal of larger BC through cloud-precipitation
processes.
The number fraction of internally mixed BC particles,
as well as the thickness of the coating on the BC core(evaluated at ~ 200 nm BC core size), showed marked
contrast between fresh urban plumes and fresh biomassburning plumes: Thickly coated BC particles are far more
dominant in biomass-burning plumes (Schwarz et al.
2008b; Kondo et al. 2011a). The thickness of the coating on BC particles in a fresh urban plume was found toincrease with the production of secondary aerosols (e.g.,sulfate and organics) as the plume ages in the atmosphere (Moteki et al. 2007; Shiraiwa et al. 2007; Miyakawa
et al. 2017). The average coating thickness (evaluatedat ~ 200 nm BC core diameter) was larger in the upper
troposphere to lower stratosphere than in the lower-tomiddle troposphere (Schwarz et al. 2008a). BC coating
thickness over the Arctic region, dominated by a mixture of aged and cloud-processed aerosols, was approximately independent of altitude from the surface to ~ 5 km
(Kodros et al. 2018; Ohata et al. 2021b). The degree ofinternal mixing of BC tends to be positively correlatedwith the total aerosol mass to BC mass ratio, which is anindicator of secondary aerosol production in the urban
plume or the degree of contribution of the biomass-burning plume (Schwarz et al. 2008a, b; Moteki et al. 2014).
Moteki et al. (2014) developed a method to classify themorphology of BC-containing particles into coated typeand attached type according to the single-particle LII

Moteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

signals. They found that the number fraction of attachedtype was only ~ 1% even in fresh urban air (Adachi et al.
2016), suggesting that the attached-type BC-containing
particles are negligible in the atmosphere. Recent reanalyses of worldwide ground-based observation datasets revealed that the coating thickness of BC-containing
particles universally follows exponential distributions,the parameters of which were pretty independent of BC
core size and location (Wang et al. 2022). This suggests
a possibility of a succinct but accurate representation of
the BC mixing state in global aerosol models.
Observational results on microphysical properties of
BC-containing particles obtained by the single-particle
LII have been used for testing the recent aerosol models
that explicitly simulate the BC aging process (Oshima
et al. 2009; Matsui et al. 2013; Oshima and Koike 2013).
Simulation accuracy of particle-size distribution andmixing state of BC is of fundamental importance for predicting atmospheric BC burden and its radiative effects,
as the aging and cloud-droplet activation parameterizations are considered to be significant sources of uncertainty (Textor et al. 2006; Vignati et al. 2010; Moteki et al.
2019; Yu et al. 2019a, b; Holopainen et al. 2020; Matsui
and Moteki 2020).
The new observational results obtained by the singleparticle LII have also been used for updating the aerosol
optical models for remote sensing algorithms (Schuster
et al. 2022).
3.2 Comparison of single‑particle LII with other BC
measurements

The thermal-optical and filer-based light absorption
methods were two primary techniques used for measuring BC mass concentration in ambient air, snow, andice samples before the invention of single-particle LII.
A notable advantage of thermal-optical and filter-based
light absorption methods compared with the singleparticle LII is their applicability to BC samples withany particle-size range. Pileci et al. (2021) reported
that ambient-mass concentrations of refractory carbon
derived from thermal-optical and single-particle LII
methods could differ within a factor of ~ 2. The BC measurement bias in filter-based light absorption methods canbe largely suppressed by removing volatile aerosol components using a heated aerosol inlet (Kondo et al. 2009;
Irwin et al. 2013; Ohata et al. 2019), as demonstrated in
fresh urban pollutions (Kondo et al. 2011b) and Arctic
atmosphere (Ohata et al. 2021a).
3.3 Anthropogenic iron oxide

The in situ aerosol measurements using single-particle
LII and laboratory analyses of collected aerosol samples using a transmission electron microscope (TEM)

Page 8 of 16

revealed that anthropogenic light-absorbing iron oxides(FeOx) consisting of an aggregate of magnetite nanoparticles are ubiquitous in the urban plumes and the East
Asian and Arctic troposphere (Moteki et al. 2017; Ohataet al. 2018; Yoshida et al. 2018). The mass mixing ratio ofanthropogenic FeOx in these regions was ~ 20–60% of BC(Yoshida et al. 2020). The anthropogenic FeOx aerosol islikely ubiquitous in the global troposphere (Lamb et al.
2021) and will be one of the contributors to regionalto-global-scale aerosol’s shortwave absorption (Moteki
et al. 2017; Matsui et al. 2018; Ito et al. 2018). These newobservation data provided further evidence to constrain
the magnitude and spatial distribution of anthropogenic
Fe emission (Rathod et al. 2020; Liu et al. 2022), which isan essential factor for investigating the effects of Fe-bearing aerosols on ocean fertilization (Hamilton et al. 2020;
Ito et al. 2021).
3.4 BC refractive index

The complex refractive index m = mr + imi is possibly
the most critical climate-relevant property of atmospheric aerosols as it largely determines the efficiency ofabsorption and scattering of solar radiation by particles.
Refractive indices of non-light-absorbing aerosol materials (e.g., sulfate, organics, aluminosilicates, sea salt) at
visible wavelengths are around mr ~1.5 ± 0.05 under dry
conditions. By contrast, refractive indices of insoluble
light-absorbing materials (BC, iron oxides, insoluble BrC)
are still not sufficiently known.
Experimental determination of the refractive index ofa particulate material always requires a close comparison between rigorous light-scattering theory and accurate optical measurements. The theory-to-measurementcomparisons have been technically challenging for BC
aggregates in the atmosphere due to their wavelengthscale irregularity of particle shape and mixing with otheraerosol components.
Currently, assumptions of BC refractive index at visible wavelengths are mostly chosen between the lower
and upper limits recommended by Bond and Bergstrom(2006), 1.75 + 0.63i (BB06-l) and 1.95 + 0.79i (BB06-h),respectively. The recommendation was based on a compilation of experimental results for synthetic BC samples(e.g., propane–oxygen flame soot, carbon black) obtained
earlier than the early-2000s. The validity of the BB06 isstill being determined as experimental methods in theearly-2000s include various assumptions (e.g., spherical
BC shape). The refractive index of atmospheric BC material could be variable and different from any synthetic
carbon material.
Liu et al. (2020b) pointed out that the theoreticallycomputed mass absorption cross section (MAC, ­m2/g)of uncoated BC aggregates using BB06 refractive indicesMoteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

underestimated the experimental MAC values by ~ 30%.
This systematic discrepancy suggests that further investigations on BC refractive index are still needed.
Moteki (2020) proposed a method for estimating therefractive index of waterborne particles from the measured distribution in complex forward-scattering amplitude S(0°). Moteki et al. (2023) improved this approach
using an updated S(0°)-measurement protocol (Moteki2021) and a more sophisticated inverse-scattering modelfor BC aggregates. They applied the method to constrain the ambient BC refractive index collected fromthe atmosphere over the northwestern Pacific Ocean at
633 nm wavelength. From the new S(0°) data for atmospheric BC and recently reported MAC values for various
types of flame-generated BC, Moteki et al. (2023) constrained a plausible (mr, mi) domain that contains the BC
refractive index at 633 nm wavelength:0.51 + 0.014m5.2
r ≤ mi ≤ 2.5mr − 3.5 if 1.7 ≤ mr ≤ 1.8
0.51 + 0.014m5.2
r ≤ mi ≤ 1.5 if 1.8 < mr ≤ 2.2.
Even though the BB06 values are currently “accepted”
in the climate and atmospheric science community,
they are located outside the plausible (mr, mi) domain
constrained from the new experimental evidence. The
persistent ~ 30% underpredictions of MAC using theBB06-l or BB06-h value pointed out by Liu et al. (2020b)

mi

The plausible(mr , mi) domain foratmospheric BC

The domain consistent
with measured MAC
for flame-generated
BCs
BB06-h
BB06-lA recommended value
for practical uses:(1.95, 0.96)

The domain consistent withmeasured S(0 ) for atmospheric BC
collected into water

mrFig. 2 Illustrating the three-different (mr, mi) domains for thecomplex refractive index of BC.: 1) The domain consistent withmeasured S(0°) for atmospheric BC (enclosed by black-dashedlines), 2) the domain consistent with measured MAC for various
flame-generated BCs (red-filled area), and 3) the domain constrainedby both MAC- and S(0°)-measurements (Moteki et al. 2023).
The conventional assumptions BB06-l (1.75 + 0.63i) and BB06-h(1.95 + 0.79i) (gray-filled circles) and the recommendable value forpractical uses 1.95 + 0.96i (blue-filled circle) suggested by Moteki et al.
(2023) are also plotted

Page 9 of 16

will be mitigated if its imaginary part is increased to avalue inside the suggested (mr, mi) domain.
For straightforward applications of the new constraintof BC refractive index by climate and atmosphericresearch, Moteki et al. (2023) suggested a recommendable mr + mi value from the constrained (mr, mi) domain,
1.95 + 0.96i, which was determined by increasing theimaginary part of the BB06-h to the lower mi boundaryof the plausible (mr, mi) domain (Fig. 2). Assuming the1.95 + 0.96i instead of the BB06-h (1.95 + 0.79i) will resultin a ~ 16% increase of calculated shortwave absorption
by BC-containing aerosols. This implies a non-negligible
underestimate of shortwave absorption by black carbon
aerosols in current climate simulations using BB06-h.

4 Open problems and suggestions
4.1 BC measurement techniques

The most important open issue of the current singleparticle LII technique is the uncertainty or difficultyof measuring BC particles much larger than the visible wavelengths. Current commercial single-particle
LII instruments (e.g., SP2 from Droplet Measurement
Technologies, Inc.) are designed to detect BC core
within ~ 70–500 nm volume-equivalent diameter. The
NOAA SP2 instruments used for global-scale aircraft
observations were intended to measure ~ 70–550 nm BC
core (Schwarz et al. 2010; Katich et al. 2018). Aircraft andground observations using the single-particle LII instrument of The University of Tokyo (a modified version of
SP2; Moteki and Kondo 2010), which detects 70–850 nm
BC core, indicated a non-negligible contribution of BC
with >  ~ 500 nm diameter to size-integrated BC mass
mixing ratio (Kondo et al. 2016; Yoshida et al. 2020). Thisimplies the significance of extending the upper limit of
the BC core size range observable by single-particle LII
instruments at least up to ~ 1000 nm. The importance ofextending the LII-detectable particle-size range is evenmore evident for FeOx (Moteki et al. 2017; Lamb et al.
2021). The author therefore suggests fundamental investigations for extending the upper limit of the observableparticle-size range in the single-particle LII.
Another important open issue on the current BC measurement technique is the lack of measurement principles
applicable to various types of sample fluids. For example,
single-particle LII is currently not able to apply to the BC
particles suspended in high-solute concentration fluids
such as ocean water. One of the unique advantages of
the CAS compared with single-particle LII is its applicability to in situ single-particle measurements of any
insoluble particles suspended in any transparent liquids(e.g., freshwater, ocean water, organic solvents). The CAS
is a potential tool for in situ real-time measurements of
BC in ocean water. In addition, the CAS will be able toMoteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

measure both BC and mineral dust particles coexistingin an environmental water sample (Yoshida et al. 2022).
The author suggests investigations on CAS technique tobe able to use it for in-line measurement of size-resolved
number concentrations of BC particles in various typesof environmental fluids. Before the wide applications,consistencies in the quantified physical properties (e.g.,
BC mass) between single-particle LII and CAS should
also be established.
4.2 BC outside the troposphere

Observational understandings of BC outside the troposphere still need to be improved. BC exerts stronger radiative effects per unit mass in the stratosphere than in the
troposphere due to its longer lifetime and higher actinic
flux. It was known that biomass-burning (BB) plumes
from wildfires could penetrate the tropopause andintrude into the lower stratosphere through strong convective systems (Jost et al. 2004; Ansmann et al. 2018).
Sporadic intrusions of BB plumes enhance the annual
mean BC mass mixing ratio of the lowermost stratosphere over Europe and North America by about ~ 75%from the regional background (Ditas et al. 2018). Strong
shortwave absorption by BC drives buoyant uplift of
the injected plumes in the stratosphere (Yu et al. 2019b,
2021; Gao et al. 2021). Further understanding of the origins, physicochemical properties, and removal processesof stratospheric aerosols are needed (Kremser et al. 2016;
Murphy et al. 2021) to predict the effects and side-effectsof the stratospheric aerosol injection for solar radiation
management (e.g., Niemeier and Timmreck 2015). The
author suggests that in situ BC measurements in thestratosphere help to develop the fundamental understanding as BC is an inert particle tracer of combustionoriginated tropospheric materials.
BC in the cryosphere has been actively investigatedfor its importance as a climate forcer and as a proxy ofhistorical environmental changes (Kang et al. 2020). BC
embedded in the ice sheets can provide information on
the historical record of atmospheric concentration of
combustion-induced aerosols (e.g., McConnell et al.
2007; Winstrup et al. 2019). BC significantly contributes
to snow albedo reduction in polar regions and midlatitude glaciers (Flanner et al. 2007; Skiles et al. 2018). It
was estimated that BC is the second largest contributor
to positive radiative forcing among all the anthropogenic
gases and aerosols in Arctic regions due mainly to its
effects on snow albedo reduction (Oshima et al. 2020).
However, the interpretation of BC-in-snow observations is still controversial due to the complex processes
that affect BC concentration and microphysical properties after deposition (e.g., Schmitt et al. 2019). Particlesize distribution of BC-in-snow and BC-in-glacier tends

Page 10 of 16

to be substantially larger than the BC-in-atmosphere
for unknown physical mechanisms (Schwarz et al. 2013;
Zhang et al. 2017; Mori et al. 2019; Kinase et al. 2020).
The larger shift of BC size distribution might cause anunderestimate of BC mass concentration measured bysome commercial single-particle LII instruments without extending the detectable BC size range. The author
suggests the importance of further improvements of BC
measurement techniques for snow and ice-sheet samples
in terms of accuracy and ease of operation. That should
help to accelerate understanding of the physical properties and processes of BC in the cryosphere.
BC is persistent in the natural environment on timescales of centuries to millennia (Goldberg 1985). Occurrences of wildfires and burnings of fossil fuel and biofuel
modify the turnover rate of the global carbon cycle byconverting relatively labile organic carbon to more environmentally persistent, slowly cycling BC (Coppola et al.
2022). A large fraction of BC particles emitted into theatmosphere will be input into the ocean. BC is the largest
slow-cycling organic carbon reservoir in the ocean (e.g.,
Yamashita et al. 2022). The current standard analyticalmethods for BC in ocean water were designed to quantify
the dissolved refractory aromatic molecules (dissolvedBC) (e.g., Dittmar 2008), which is different from the analytical methods for particulate BC in the atmosphere(Coppola et al. 2022). A quantitative estimate of the oceanic BC budget requires atmospheric BC data (Bao et al.
2017). However, the consistency of the current BC datasets available from atmospheric and oceanic disciplines
is nearly unknown. The author suggests that the CAS
would help to provide consistent particulate BC datasetsin the atmosphere, cryosphere, and ocean.

5 Conclusive remarks
We reviewed recent advances in in situ measurement
methods and observational findings since the mid-2000s
on atmospheric BC aerosol, one of the most important
short-lived climate forcers. Quantification of climate-relevant properties of atmospheric BC and BC-containing
particles has been continually updated over two decades.
The single-particle LII has been playing an important rolein field observations and observation-based updates ofassumptions in climate models and remote sensing algorithms. Although the global anthropogenic BC emission
from fossil fuel burning is expected to decrease owing
to the clean air act, natural BC emissions from wildfires
and the occurrence of BC injection to the stratosphere
may increase globally with greenhouse gas-induced climate change. Further developments in the measurement
methods and observational knowledge on environmental
BC should help improve the predictabilities of short-termMoteki ﻿Progress in Earth and Planetary Science 2023, 10(1):12

climate response to atmospheric composition and thelong-term global carbon cycle.
Abbreviations
BC	Black carbon
BrC	Brown carbon
OC	Organic carbon
FeOx	Iron oxides
LII	Laser-induced incandescenceSP2	Single-particle soot photometerCAS	Complex amplitude sensor
Acknowledgements
The author acknowledges the Japan Geoscience Union for this opportunity towrite a review paper focused on the author’s research area.
Author contributions
NM conceived the research idea and wrote the manuscript. The author readand approved the final manuscript.
Funding
Funds were provided by the Environment Research and Technology Development Fund (JPMEERF20202003) of the Environmental Restoration and Conservation Agency, the Japan Society for the Promotion of Science (JSPS) KAKENHI
program (JP19H04236, JP19KK0289, JP19H04259, JP19H05699, 22H03722,
and 22H01294), and the Arctic Challenge for Sustainability ArCS II project(JPMXD1420318865) of the Ministry of Education, Culture, Sports, Science, andTechnology (MEXT) of Japan.
Availability of data and materials
Not applicable.

Declarations
Competing interests
The authors declare that they have no competing interests.
Received: 11 January 2023 Accepted: 28 February 2023
Published: 6 March 2023

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