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Black carbon (BC) particles in the Arctic contribute to rapid warming of the Arctic by heating the atmosphere and snow and ice surfaces. Understanding the source contributions to Arctic BC is therefore important, but they are not well understood, especially those for atmospheric and snow radiative effects. Here we estimate simultaneously the source contributions of Arctic BC to near-surface and vertically integrated atmospheric BC mass concentrations (MBC_SRF and MBC_COL), BC deposition flux (MBC_DEP), and BC radiative effects at the top of the atmosphere and snow surface (REBC_TOA and REBC_SNOW), and show that the source contributions to these five variables are highly different. In our estimates, Siberia makes the largest contribution to MBC_SRF, MBC_DEP, and REBC_SNOW in the Arctic (defined as > 70° N), accounting for 70 %, 53 %, and 43 %, respectively. In contrast, Asia’s contributions to MBC_COL and REBC_TOA are largest, accounting for 38 % and 45 %, respectively. In addition, the contributions of biomass burning sources are larger (24−34 %) to MBC_DEP, REBC_TOA, and REBC_SNOW, which are highest from late spring to summer, and smaller (4.2−14 %) to MBC_SRF and MBC_COL, whose concentrations are highest from winter to spring. These differences in source contributions to these five variables are due to seasonal variations in BC emission, transport, and removal processes and solar radiation, as well as to differences in radiative effect efficiency (radiative effect per unit BC mass) among sources. Radiative effect efficiency varies by a factor of up to 4 among sources (1465−5439 W g–1) depending on lifetimes, mixing states, and heights of BC and seasonal variations of emissions and solar radiation. As a result, source contributions to radiative effects and mass concentrations (i.e., REBC_TOA and MBC_COL, respectively) are substantially different. The results of this study demonstrate the importance of considering differences in the source contributions of Arctic BC among mass concentrations, deposition, and atmospheric and snow radiative effects for accurate understanding of Arctic BC and its climate impacts.

Black carbon is the largest contributor to global aerosol’s shortwave absorption in the current atmosphere and is an important positive climate forcer. The complex refractive index, m = mr + imi, the primary determinant of the absorbed and scattered energies of incident radiation per unit volume of particulate material, has not been accurately known for atmospheric black carbon material. An accurate value at visible wavelengths has been difficult to obtain due to the black carbon’s wavelength-scale irregularity and variability of aggregate shape, distribution in particle size, and mixing with other aerosol compounds. Here, we present a method to constrain a plausible (mr, mi) domain for black carbon from the observed distribution of the complex forward-scattering amplitude S(0°). This approach suppresses the biases due to the above-mentioned complexities. The S(0°) distribution of black carbon is acquired by performing single particle S(0°) measurements in a water medium after collecting atmospheric aerosols into water. We demonstrate the method operating at λ = 0.633 μm for constraining the refractive index of black carbon aerosols in the north-western Pacific boundary layer. From the plausible (mr, mi) domain consistent with the observed S(0°) distributions and the reported range of mass absorption cross-section, we conservatively select 1.95 + 0.96i as a recommendable value of the refractive index for uncoated black carbon at visible wavelengths. The recommendable value is 0.17 larger in mi than the widely used value 1.95 + 0.79i in current aerosol-climate models, implying a ∼16% underestimate of shortwave absorption by black carbon aerosols in current climate simulations.

An accurate observational dataset of the size-resolved concentration of mineral dust particles in the atmosphere, hydrosphere, and cryosphere is needed for investigating the effect of mineral dust on the climate with earth system models. However, automated measurements of dust particles remain challenging due to the complexities of the physicochemical properties (e.g., shape and mineralogy) of individual dust particles and the difficulties in discriminating dust from other particulate components (e.g., black carbon). Here, we suggest the use of complex forward-scattering amplitude data obtained by the single particle extinction and scattering (SPES) method as a low-cost optical approach for identification and quantification of silicate (aluminosilicates + quartz) particles, the major particulate component of desert dust. We focus here on the submicron particle-size range to challenge the robust identification of wavelength or smaller scale dust solely according to the principle of elastic light scattering. The two-dimensional nature of the complex scattering amplitude data allows us to identify silicate-dominant particles in waterborne dust samples and discriminate them from light-absorbing particulate components (e.g., hematite). We demonstrate that the two-dimensional dataspace of the complex amplitude allows an accurate retrieval of the particle-size distribution of silicate particles thanks to the simultaneous retrieval of the particle’s effective refractive index. We discuss some notable differences in our results from those retrieved from conventional elastic light scattering approaches. Copyright © 2022 American Association for Aerosol Research

During the PAMARCMiP 2018 campaign (March and April 2018) a proton-transfer-reaction mass spectrometer (PTR-MS) was deployed onboard the POLAR 5 research aircraft and sampled the high Arctic atmosphere under Arctic haze conditions. More than 100 compounds exhibited levels above 1 pmol/mol in at least 25 % of the measurements. We used back trajectories and acetone mixing ratios to identify periods with and without long-range transport from continental sources. Air masses with continental influence contained elevated levels of compounds associated with aged biogenic emissions and anthropogenic pollution (e.g., methanol, peroxyacetylnitrate (PAN), acetone, acetic acid, methylethylketone (MEK), proprionic acid, and pentanone). Almost half of all positively detected compounds (> 100) in the High Arctic atmosphere can be associated with terpene oxidation products. This may constitute a signature of biogenic terpenes and their oxidation products on the high Arctic atmosphere. Many of these compounds will condense and produce biogenic secondary organic aerosol (SOA) – a natural source of organic aerosol (OA) in addition to the aerosols that can be associated with pollution. Therefore, we hypothesize that biogenic SOA may have exerted significant control over the complex system of aerosols, clouds and longwave radiation in the pre-industrial Arctic winter, even though their role is likely marginal under contemporary polluted Arctic haze conditions. However, biogenic SOA may become an important factor in the futRure again, if biogenic emissions are enhanced due to climate change and if polluting technologies are phased out in the future. During two flights, surface ozone depletion events (ODE) were observed that coincided with enhanced levels of acetone, and methylethylketone. There is evidence that ODEs may also be associated with the emission of biogenic ice-nucleating particles (INP) because the filter samples taken during these two flights exhibited enhanced levels of highly active INP. Both these processes, INP production in association with ozone depletion events, and the transport of biogenic SOA could require corrections in estimates of Arctic change. If the preindustrial effects from these natural factors was stronger than is thought, subsequent climate changes over the Arctic may be larger than currently assumed.

Key Points: • First ever measurements with a high‐accuracy single‐particle soot photometer of black carbon (BC) concentrations in Arctic snowpack • Topography and BC emission flux strongly influenced latitudinal variations of mass concentrations and size distributions of BC • Measured BC mass concentrations 2–25 times lower than previously reported show the importance of revalidating climate models Black carbon (BC) deposited on snow lowers its albedo, potentially contributing to warming in the Arctic. Atmospheric distributions of BC and inorganic aerosols, which contribute directly and indirectly to radiative forcing, are also greatly influenced by depositions. To quantify these effects, accurate measurement of the spatial distributions of BC and ionic species representative of inorganic aerosols (ionic species hereafter) in snowpack in various regions of the Arctic is needed, but few such measurements are available. We measured mass concentrations of size-resolved BC (CMBC) and ionic species in snowpack by using a single-particle soot photometer and ion chromatography, respectively, over Finland, Alaska, Siberia, Greenland, and Spitsbergen during early spring in 2012–2016. Total BC mass deposited per unit area (DEPMBC) during snow accumulation periods was derived from CMBC and snow water equivalent (SWE). Our analyses showed that the spatial distributions of anthropogenic BC emission flux, total precipitable water, and topography strongly influenced latitudinal variations of CMBC, BC size distributions, SWE, and DEPMBC. The average size distributions of BC in Arctic snowpack shifted to smaller sizes with decreasing CMBC due to an increase in the removal efficiency of larger BC particles during transport from major sources. Our measurements of CMBC were lower by a factor of ~13 than previous measurements made with an Integrating Sphere/Integrating Sandwich spectrophotometer due mainly to interference from coexisting non-BC particles such as mineral dust. The SP2 data presented here will be useful for constraining climate models that estimate the effects of BC on the Arctic climate. Plain Language Summary Black carbon (BC) particles, commonly known as soot, are emitted from incomplete combustion of fossil fuels and biomass. They efficiently absorb solar radiation and thus heat the atmosphere. BC particles emitted at midlatitudes and in the Arctic are deposited onto snow in the Arctic, accelerating snowmelt in early spring by absorbing solar radiation. These processes contribute to warming in the Arctic. Calculations of this warming effect by using numerical models need to be validated by comparison with observed BC concentrations in snowpack. However, there are very few accurate records of concentrations of BC in snow because of technical difficulties in making these measurements. We developed a new laser-induced incandescence technique to measure BC concentrations in snowpack and applied it for the first time in six Arctic regions (Finland, Alaska, North and South Siberia, Greenland, and Spitsbergen). The BC concentrations we measured were highest in Finland and South Siberia, which are closer to large anthropogenic BC sources than the other regions, where our measured BC concentrations were much lower. On average, our BC concentrations were much lower than those previously measured by different techniques. Therefore, previous comparisons of modeled and observed BC concentrations need to be re-evaluated using the present data.

Long-term measurements of black carbon (BC) aerosols by filter-based absorption photometers with a heated inlet (COSMOS) in different regions have been useful in elucidating spatial variati...

Black carbon (BC) aerosol deposited in and onto Arctic snow increases the snow's absorption of solar radiation and accelerates snowmelt. Concentrations of BC in the Arctic atmosphere and snow are controlled by wet deposition; however, details of this process are poorly understood owing to the scarcity of time-resolved measurements of BC in hydrometeors. We measured mass concentrations of BC in hydrometeors (CMBC) and in air (MBC) with 16% and 15% accuracies, respectively, at Ny-Ålesund, Svalbard during 2012–2019. Median monthly MBC and CMBC values showed similar seasonal variations, being high in winter-spring and low in summer. Median monthly BC wet deposition mass flux (FMBC) was highest in winter and lowest in summer, associated with seasonal patterns of CMBC and precipitation. Seasonally averaged BC size distributions in hydrometeors were similar except for summer. Measurements of MBC and CMBC in spring 2017 showed a size-independent removal efficiency, indicating that BC-containing particles were efficiently activated into cloud droplets. These observations at Ny-Ålesund were compared with observations at Barrow, Alaska, during 2013–2017. The near-surface MBC at Ny-Ålesund and Barrow had similar seasonal patterns; however, the two sites differed in CMBC and FMBC. In summer, CMBC was low at Ny-Ålesund but moderate at Barrow, likely reflecting differences in MBC in the lower troposphere. Seasonally averaged BC size distributions in hydrometeors were similar at both sites, suggesting that average BC size distributions are similar in the Arctic lower troposphere. The efficiency of BC removal tends to be size-independent during transport, leading to the observed similarity.

Long-term measurements of black carbon (BC) are warranted for investigating changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including multi-angle absorption photometers (MAAP), particle soot absorption photometers (PSAP), continuous light absorption photometer (CLAP), and Aethalometers. The measured babs can be converted to atmospheric mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC = babs/MBC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS-derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2) and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC, and long-term stability of the correlation slope, which represents the MAC. In general, babs – MBC (COSMOS) correlations were high (r2 = 0.84–0.96 for hourly data) at Fukue in Japan, Barrow in Alaska, Ny-Ålesund in Svalbard, Pallastunturi in Finland, and Alert in Canada, and stable up to for 10 years. We successfully estimated MAC values (11.0–15.2 m2 g−1 at a wavelength of 550 nm) for these instruments and these MAC values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC in these Arctic sites estimated by this method are consistent with each other, they are applicable to study spatial and temporal variation of MBC and to evaluate performance of numerical model calculations.

The 11th Symposium on Polar Science/Ordinary sessions: [OM] Polar Meteorology and Glaciology, Thu. 3 Dec.

The 11th Symposium on Polar Science/Special session: [S] Accelerating Arctic research: Recent progress and future prospect of Arctic research, Tue. 1 Dec.

Black carbon (BC) particles cause adverse health effects and contribute to the heating of the atmosphere by absorbing visible solar radiation. Efforts have been made to reduce BC emissions, especially in urban areas; however, long-term measurements of BC mass concentration (MBC) are very limited in Japan. We report MBC measurements conducted in Tokyo from 2003 to 2017, showing that MBC decreased by a factor of 3 from 2003 to 2010 and was stable from 2010 to 2017. Fine particulate concentrations (PM2.5) decreased by a much smaller factor during 2003–2010. The diurnal variations of BC size distributions suggest that the BC in Tokyo originates mainly from local sources, even after 2010. Our three-dimensional model calculations show that BC from the Asian continent contributes a small portion (about 20%) of the annual average MBC in the Kanto region of Japan, which includes Tokyo. This indicates that continued reduction of BC emissions inside Japan should be effective in further decreasing MBC.

The Tenth Symposium on Polar Science/Ordinary sessions: [OM] Polar Meteorology and Glaciology, Thu. 5 Dec. / 2F Auditorium , National Institute of Polar Research

Atmospheric iron affects the global carbon cycle by modulating ocean biogeochemistry through the deposition of soluble iron to the ocean. Iron emitted by anthropogenic (fossil fuel) combustion is a source of soluble iron that is currently considered less important than other soluble iron sources, such as mineral dust and biomass burning. Here we show that the atmospheric burden of anthropogenic combustion iron is 8 times greater than previous estimates by incorporating recent measurements of anthropogenic magnetite into a global aerosol model. This new estimation increases the total deposition flux of soluble iron to southern oceans (30–90 °S) by 52%, with a larger contribution of anthropogenic combustion iron than dust and biomass burning sources. The direct radiative forcing of anthropogenic magnetite is estimated to be 0.021 W m−2 globally and 0.22 W m−2 over East Asia. Our results demonstrate that anthropogenic combustion iron is a larger and more complex climate forcer than previously thought, and therefore plays a key role in the Earth system., As a source of soluble iron, anthropogenic combustion iron is considered less important than natural sources. Here, the authors combine new measurements with a global aerosol model and show the atmospheric burden of anthropogenic combustion iron to be 8 times greater than previous estimates.

Theoretical and experimental bases are given for measuring the complex forward-scattering amplitude of single particles through self-reference interferometry. Our analyses reveal the nondimensional parameters that primarily control the accuracy and resolution of the complex amplitude data. We propose a measurement protocol, Complex Amplitude Sensing version 1 (CAS-v1), for effectively utilizing self-reference interferometry as a universal tool for inline measurements of the complex forward-scattering amplitude of single sub- and super-micron particles suspended in a fluid flow. The CAS-v1 protocol will facilitate applications of self-reference interferometry to real-time particle measurements in the industrial, biomedical, and environmental sciences.

Long-term measurements of the light absorption coefficient (b(abs)) obtained with a particle soot absorption photometer (PSAP), b(abs) (PSAP), have been previously reported for Barrow, Alaska, and ...

Quantitative simulation of an aerosol’s lifecycle by regional-scale and global-scale atmospheric models is mandatory for unbiased analysis and prediction of aerosol radiative forcing and climate change. Globally, aerosol deposition is dominated by the rainout process, which is mostly triggered by activation of aerosols to liquid droplets in supersaturated domains of precipitating clouds. However, the actual environmental supersaturation value that aerosols experience in precipitating clouds is difficult for models to predict, and it has never been constrained by observations; as a result, there is large uncertainty in atmospheric aerosol simulations. Here, by a particle-tracer analysis of 37 rainfall events in East Asia, near the largest source region of anthropogenic aerosols in the northern hemisphere, we observed that the environmental supersaturation actually experienced by the removed aerosols in precipitating clouds averaged 0.08 ± 0.03% and ranged from 0.03 to 0.2%. Simulations by a mixing-state-resolved global aerosol model showed that the simulated long-range transport efficiency and global atmospheric burden of black carbon aerosols can be changed by a factor of two or three as a result of a change in the environmental supersaturation in precipitating clouds within just 0.08 ± 0.03%. This result is attributable to the fact that the sensitivity of an aerosol’s rainout efficiency to environmental supersaturation is higher for the less-aged black carbon concentrated near source regions. Our results suggest that observational constraints of environmental supersaturation in precipitating clouds, particularly near source regions, are of fundamental importance for accurate simulation of the atmospheric burden of black carbon and other aerosols. A delicate balance determines whether or not precipitation will generate the rainout, or removal, of atmospheric aerosols. The process is critical for climate and human health, but is only approximately simulated in most models. A multi-institution team led by Nobuhiro Moteki from the University of Tokyo has quantified the cloud supersaturation conditions that are required to generate ‘nucleation scavenging’, the mechanism ultimately leading to aerosol rainout. By measuring black carbon aerosols in surface air before convective precipitation and comparing it to aerosols within the precipitation itself, the team established that rainout occurred with supersaturation of about 0.08%. The threshold, however, was lower for hydrophilic, older aerosols and higher for hydrophobic, younger aerosols. Using a global aerosol model, the research shows that the high threshold in young aerosols reduces rainout near emission sources and enhances atmospheric transport of aerosols to distant regions.

The Ninth Symposium on Polar Science/Ordinary sessions: [OM] Polar meteorology and glaciology, Wed. 5 Dec. / 3F Multipurpose Conference room, National Institute of Polar Research

Aerosols and clouds play important roles in the Arctic climate. Conversely, aerosol emissions and cloud formation are affected by changes in the Arctic climate. This paper reviews studies of aerosols and clouds performed during the Arctic Challenge for Sustainability (ArCS) project carried out by the National Institute of Polar Research (NIPR) in Japan and collaborating institutions. The ArCS project included intensive studies of black carbon aerosols (BC). We installed Continuous Soot Monitoring System (COSMOS) instruments to measure atmospheric BC at four locations in the Arctic, establishing the Arctic BC COSMOS Measurement Network (ABCM-net). We also measured BC concentrations in snowpack in extensive areas of the Arctic and showed that previous studies have greatly overestimated BC in snowpack. We developed and improved new aerosol models that achieved better agreements with measurements of BC in the Arctic atmosphere, snowpack, and falling snow. We made new estimates of radiative forcing of BC in the Arctic atmosphere and snow/ice surfaces that lower their albedo. In addition to these researches on BC, we made accurate measurements of ice nucleating particles (INPs) at Ny-Alesund, Svalbard, showing that their concentrations increased in summer as a result of dust particle emissions from glacial outwash sediments. This high ice nucleating ability was likely due to the presence of organic substances mixed with the dust particles. We also made continuous cloud radar measurements and the first continuous in-situ measurements of cloud microphysical properties in the Arctic at Ny-Alesund. Results from these cloud measurements and their relationship with aerosols are described.

Light-absorbing atmospheric aerosols such as carbonaceous particles influence the climate through absorbing sunlight. The mixing states of these aerosol particles affect their optical properties. This study examines the changes in the mixing states and abundance of strongly light-absorbing carbonaceous particles by using transmission electron microscopy (TEM) and single-particle soot photometer (SP2), as well as of iron-oxide particles, in Tokyo, Japan. TEM and SP2 use fundamentally different detection techniques for the same light-absorbing particles. TEM allows characterization of the morphological, chemical, and structural features of individual particles, whereas SP2 optically measures the number, size, and mixing states of black carbon (BC). A comparison of the results obtained using these two techniques indicates that the peaks of high soot (nanosphere soot (ns-soot)) concentration periods agree with those of the BC concentrations determined by SP2 and that the high Fe-bearing particle fraction periods measured by TEM agree with that of high number concentrations of iron-oxide particles measured using SP2 during the first half of the observation campaign. The results also show that the changes in the ns-soot/BC mixing states primarily correlate with the air mass sources, wind speed, precipitation, and photochemical processes. Nano-sized, aggregated, iron-oxide particles mixed with other particles were commonly observed by using TEM during the high-iron-oxide particle periods. We conclude that, although further quantitative comparison between TEM and SP2 data will be needed, the morphologically and optically defined ns-soot and BC, respectively, are essentially the same substance and that their mixing states are generally consistent across the techniques.

An accurate and efficient simulation of light scattering by an atmospheric black carbon (BC)-containing aerosol—a fractal-like cluster of hundreds of carbon monomers that is internally mixed with other aerosol compounds such as sulfates, organics, and water—remains challenging owing to the enormous diversities of such aerosols׳ size, shape, and mixing state. Although the discrete dipole approximation (DDA) is theoretically an exact numerical method that is applicable to arbitrary non-spherical inhomogeneous targets, in practice, it suffers from severe granularity-induced error and degradation of computational efficiency for such extremely complex targets. To solve this drawback, we propose herein a hybrid DDA method designed for arbitrary BC-containing aerosols: the monomer-dipole assumption is applied to a cluster of carbon monomers, whereas the efficient cubic-lattice discretization is applied to the remaining particle volume consisting of other materials. The hybrid DDA is free from the error induced by the surface granularity of carbon monomers that occurs in conventional cubic-lattice DDA. In the hybrid DDA, we successfully mitigate the artifact of neglecting the higher-order multipoles in the monomer-dipole assumption by incorporating the magnetic dipole in addition to the electric dipole into our DDA formulations. Our numerical experiments show that the hybrid DDA method is an efficient light-scattering solver for BC-containing aerosols in arbitrary mixing states. The hybrid DDA could be also useful for a cluster of metallic nanospheres associated with other dielectric materials.

An improved understanding of the variations in the mass concentration and size distribution of black carbon (BC) in the free troposphere (FT) over East Asia, where BC emissions are very high, is needed to reliably estimate the radiative forcing of BC in climate models. We measured these parameters and the carbon monoxide (CO) concentration by conducting the Aerosol Radiative Forcing in East Asia (A-FORCE) 2013W aircraft campaign in East Asia in winter 2013 and compared these data with measurements made in the same region in spring 2009. The median BC concentrations in the FT originating from North China (NC) and South China (SC) showed different seasonal variations, which were primarily caused by variations in meteorological conditions. CO concentrations above the background were much higher in SC than in NC in both seasons, suggesting a more active upward transport of CO. In SC, precipitation greatly increased from winter to spring, leading to an increased wet deposition of BC. As a result, the median BC concentration in the FT was highest in SC air in winter. This season and region were optimal for the effective transport of BC from the planetary boundary layer to the FT. The count median diameters of the BC size distributions generally decreased with altitude via wet removal during upward transport. The altitude dependence of the BC size distributions was similar in winter and spring, in accord with the similarity in the BC mixing state. The observed BC concentrations and microphysical properties will be useful for evaluating the performance of climate models.

Atsushi Yoshida, Nobuhiro Moteki, Sho Ohata, Tatsuhiro Mori, Ryuji Tada, Pavla Dagsson-Waldhauserov a, and Yutaka Kondo Department of Earth and Planetary Science, The University of Tokyo, Tokyo, Japan; Faculty of Environmental Sciences, Agricultural University of Iceland, Hvanneyri, Iceland; Faculty of Physical Sciences and Faculty of Earth Sciences, University of Iceland, Reykjav ik, Iceland; Faculty of Environmental Sciences, Czech University of Life Sciences Prague, Prague, Czech Republic; Meteorology and Glaciology Group, National Institute of Polar Research, Tokyo, Japan

Black carbon (BC) aerosols become internally mixed with non-BC compounds (BC coatings) during aging in the atmosphere. In this study, we measured the hygroscopicity parameter κ on a single-particle basis for both BC-coating materials (κBC-coat) and BC-free particles (κBC-free) in the urban atmosphere of Tokyo, using a single-particle soot photometer (SP2). In our measurement system, dry ambient particles were first mass selected by an aerosol particle mass analyzer, then humidified, and then passed to the SP2 for detection of their refractory BC mass content and optical diameter. A quadrupole aerosol mass spectrometer was also employed to interpret the hygroscopicity data. During the observation period, the measured κBC-coat generally agreed with κBC-free to within ±25% and was usually in typical range for inorganic and organic aerosols. These results indicate that BC-coating materials and BC-free particles in Tokyo usually had similar chemical compositions, internal mixtures of inorganic and organic compounds, even in a source region. However, occasionally κBC-coat was much higher than κBC-free values, when the mass concentrations of BC and organic aerosols were poorly correlated. This indicates external mixing of BC-containing and BC-free particles from different sources. These findings improve our understanding of the cloud condensation nuclei activity of BC-containing particles, which strongly influences their wet removal, and optical properties in the ambient air.

To investigate the effects of the regulations of diesel and non-methane hydrocarbon (NMHCs) emissions in the Tokyo metropolitan area (TMA) on the characteristics of carbonaceous aerosols (organic carbon (OC) and elemental carbon (EC)), we conducted field observations to characterize carbonaceous aerosols in the TMA in the summer of 2004 and 2014 (the end of July-middle of August). Following the enforcement of diesel emission regulations, EC concentrations showed a four-fold decrease from 2004 to 2014. However, OC concentrations showed no significant decrease in the last decade. Multiple chemical analyses revealed the differences in the impacts of the contribution of oxygenated fraction, biogenic NMHCs on OC, and the secondary organic aerosol-Ozone relationship between 2004 and 2014. Further investigations into the emission inventory for recent years, especially in terms of precursor gases, are needed for better prediction of OC in the TMA using chemical transport models.