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Forest wildfires in interior Alaska represent an important black carbon (BC) source for the Arctic and sub-Arctic. However, BC observations in interior Alaska have not been sufficient to constrain the range of existing emissions. Here, we show our observations of BC mass concentrations and carbon monoxide (CO) mixing ratios in the Poker Flat Research Range (65.12° N, 147.43° W), located in central Alaska, since April 2016. The medians of the hourly BC mass concentration and CO mixing ratio throughout the observation period were 13 ng m-3 and 124.7 ppb, respectively. Significant peaks in the BC mass concentration and CO mixing ratio were observed at the same time, indicating influences from common sources. These BC peaks coincided with peaks at other comparative sites in Alaska, indicating large BC emissions in interior Alaska. Source estimation by FLEXPART-WRF confirmed a contribution of forest wildfires in Alaska when high BC mass concentrations were observed. For these cases, we found a positive correlation (r = 0.44) between the observed BC/CO ratio and fire radiative power (FRP) observed in Alaska and Canada. This finding indicates that the BC and CO emission ratio is controlled by the intensity and time progress of forest wildfires and suggests the BC emission factor or/and inventory could be potentially improved by FRP. We recommend that FRP be integrated into future bottom-up emission inventories to achieve a better understanding of the dynamics of pollutants from frequently occurred forest wildfires under the rapidly changing climate in the Arctic. [ABSTRACT FROM AUTHOR]

Atmospheric transport of iron (Fe) in fine anthropogenic aerosol particles is an important route of soluble Fe supply to remote oceans from continental areas. To investigate Fe properties of aerosol particles over remote oceans, we analyzed atmospheric aerosol particles over the Indian Ocean during the research vessel Hakuho Maru KH-18-6 cruise. Aerosol particles collected using a cascade impactor were analyzed using transmission electron microscopy (TEM) with an energy-dispersive X-ray spectrometry analyzer. The particle shape and composition on the sample stage of 0.3-0.8 µm aerodynamic diameter indicated that most particles collected north of the equator were composed mainly of ammonium sulfate. Regarding the particle number fraction, 0.6-3.0% of particles contained Fe, which mostly co-existed with sulfate. Of those particles, Fe was found 26% as metal spheres, often co-existing with Al or Si, regarded as fly ash, 14% as mineral dust, and 7% as iron oxide aggregations. Water-dialysis analyses of TEM samples indicated that Fe in spherical fly ash was almost entirely insoluble, whereas Fe in the other morphological-typed particles was partly (65% Fe mass on average) soluble. Global model simulations mostly reproduce observed Fe mass concentrations in PM2.5 collected using a high-volume air sampler, including their north-south contrast during the cruise. In contrast, a marked difference was found between the simulated mass fractions of Fe mineral sources and the observed Fe types. For example, the model underestimated anthropogenic aluminosilicate Fe contained in matter such as fly ash from coal combustion. Our observations suggest that Fe in particles over remote ocean areas has multiple shapes and minerals, and further suggest that its solubility after aging processes differs depending on their morphological and mineral type. Proper consideration of such Fe types at their sources is necessary for accurate estimation of atmospheric Fe effects on marine biological activity. [ABSTRACT FROM AUTHOR]

We investigated the association of marine biological indicators (polysaccharides and protein-like gel particles, Chl-a) with the formation of fluorescent aerosol particles, cloud condensation nuclei (CCN), and ice-nucleating particles (INPs) over the North Pacific Ocean, Bering Sea, and Arctic Ocean during September–November 2019. The abundance of bioindicators was high in the North Pacific Ocean and the Bering Sea (e.g., up to 1.3 mg m−3 of Chl-a), suggesting high biological activity known as the autumn bloom. In the North Pacific Ocean, particles were characterized by high mass fractions of organics and sulfate with predominance of terrestrial air masses. Conversely, in the Bering Sea and the Arctic Ocean, particles were characterized by high mass fractions of sea salt and sulfate with predominance of maritime air masses. The averaged CCN concentration at 0.4 % supersaturation ranged from 99–151, 43–139, to 36 cm−3 over the North Pacific Ocean with terrestrial influences, over the Bering Sea with marine biogenic influences, and over the Arctic Ocean with marine influences, respectively, and the corresponding range of hygroscopicity parameter ĸ was 0.17–0.60, 0.42–0.68, and 0.67, respectively. The averaged INP concentration (NINP) measured at temperatures of −18 and −24 °C with marine sources was 0.01–0.09 and 0.1–2 L−1, respectively, and that over the Arctic Ocean was 0.001–0.016 and 0.012–0.27 L−1, respectively. When marine sources were dominant, fluorescent bioaerosols were strongly correlated with all bioindicator types (R: 0.81–0.88) when considering the wind-uplifting effect from the sea surface to the atmosphere. Correlations between NINP measured at −18 and −24 °C and all bioindicator types (R: 0.58–0.95 and 0.79–0.93, respectively) and between NINP and fluorescent bioaerosols (R: 0.50 and 0.60, respectively) were also positive, suggesting that marine bioindicators contributed substantially as sources of bioaerosols and cloud formation. [ABSTRACT FROM AUTHOR]

Nitrous acid (HONO) is an important atmospheric gas given its contribution to the cycles of NOx and HOx, but its role in global atmospheric photochemistry is not fully understood. This study, for the first time, implemented three pathways of HONO formation in the chemistry-climate model CHASER (MIROC-ESM) to explore three physical phenomena: gas-phase kinetic reactions (GRs), direct emission (EM), and heterogeneous reactions on cloud/aerosol particles (HRs). We evaluated the simulations by the atmospheric measurements from the OMI (Ozone Monitoring Instrument), EANET (Acid Deposition Monitoring Network in eastern Asia) / EMEP (European Monitoring and Evaluation Programme) ground-based stationary observations, observations from the ship R/V Mirai, and aircraft-based measurements by ATom1 (atmospheric tomography) and EMeRGe-Asia-2018 (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global scales). We showed that the inclusion of the HONO chemistry in the modeling process reduces the model bias against the measurements for PM2.5, NO3-/HNO3, NO2, OH, O3, and CO, especially in the lower troposphere and the North Pacific (NP) region. We found that the retrieved global abundance of tropospheric HONO was 1.4 TgN. Of the three source pathways, HRs and EM contributed 63 % and 26 % to the net HONO production, respectively. We also observed that, reactions on the aerosol surfaces contributed larger amounts of HONO (51 %) than those on the cloud surfaces (12 %). The model exhibited significant negative biases for daytime HONO in the Asian off-coast region, compared with the airborne measurements by EMeRGe-Asia-2018, indicating the existence of unknown daytime HONO sources. Strengthening of aerosol uptake of NO2 near-surface and in the middle troposphere, cloud uptake, and direct HONO emission are all potential yet-unknown HONO sources. We also found that the simulated HONO abundance and its impact on NOx-O3 chemistry are sensitive to the yield of the heterogeneous conversion of NO2 to HONO (vs. HNO3). Inclusion of HONO reduces global tropospheric NOx (NO + NO2) levels by 20.4 %, thereby weakening the tropospheric oxidizing capacity, which in turn, increases CH4 lifetime (13 %) and CO abundance (8 %). HRs on the surfaces of cloud particles, which have been neglected in previous modeling studies, are the main drivers of these impacts. This effect is particularly salient for the substantial reductions of levels of OH (40-67 %) and O3 (30-45 %) in the NP region during summer given the significant reduction of NOx level (50-95 %). In contrast, HRs on aerosol surfaces in China (Beijing) enhance OH and O3 winter mean levels by 600-1700 % and 10-33 %, respectively, with regards to their minima in winter. Overall, our findings suggest that a global model that does not consider HONO heterogeneous mechanisms (especially HRs on cloud particle surfaces) may erroneously predict the effect of HONO in remote areas and polluted regions. [ABSTRACT FROM AUTHOR]

Iodine compounds destroy ozone (O3) in the global troposphere and form new aerosols, thereby affecting the global radiative balance. However, few reports have described the latitudinal distribution of atmospheric iodine compounds. This work reports iodine monoxide (IO) measurements over unprecedented sampling areas from Arctic to the Southern Hemisphere and spanning sea surface temperatures (SSTs) of approximately 0°C to 31.5°C. The highest IO concentrations were observed over the Western Pacific warm pool (WPWP), where O3 minima were also measured. There, negative correlation was found between O3 and IO mixing ratios at extremely low O3 concentrations. This correlation is not explained readily by the "O3-dependent" oceanic fluxes of photolabile inorganic iodine compounds, the dominant source in recent global-scale chemistry-transport models representing iodine chemistry, and rather implies that "O3-independent" pathways can be similarly important in the WPWP. The O3-independent fluxes result in a 15% greater O3 loss than that estimated for O3-dependent processes alone. The daily O3 loss rate related to iodine over the WPWP is as high as approximately 2 ppbv despite low O3 concentrations of ~10 ppbv, with the loss being up to 100% greater than that without iodine. This finding suggests that warming SST driven by climate change may affect the marine atmospheric chemical balance through iodine–ozone chemistry. [ABSTRACT FROM AUTHOR]

This study uses a chemistry-climate model CHASER (MIROC) to explore the roles of heterogeneous reactions (HRs) in global tropospheric chemistry. Three distinct HRs of N2O5, HO2, and RO2 are considered for surfaces of aerosols and cloud particles. The model simulation is verified with EANET and EMEP stationary observations, R/V MIRAI ship-based data, ATOM1 aircraft measurements, satellite observations by OMI, ISCCP, and CALIPSO-GOCCP, and reanalysis data JRA55. The heterogeneous chemistry facilitates improvement of model performance with respect to observations for NO2, OH, CO, and O3, especially in the lower troposphere. The calculated effects of heterogeneous reactions cause marked changes in global abundances of O3 (-3%), NOx (-2.2%), CO (+3.3%), and global mean CH4 lifetime (+5.9%). These global effects were contributed mostly by N2O5 uptake onto aerosols in the middle troposphere. At the surface, HO2 uptake gives the largest contributions, with a particularly significant effect in the North Pacific region (-24% O3, +68% NOx, +8% CO, and -70% OH), mainly attributable to its uptake onto clouds. The RO2 reaction has a small contribution, but its global-mean negative effect on O3 is not negligible. In general, the uptakes onto ice crystals and cloud droplets that occur mainly by HO2 and RO2 radicals cause smaller global effects than the aerosol-uptake effects by N2O5 radicals (+1.34% CH4 lifetime, +1.71% NOx, -0.56% O3, +0.63% CO abundances). Nonlinear responses of tropospheric O3, NOx, and OH to the N2O5 and HO2 uptakes are found in the same modelling framework of this study (푅> 0.93). Although all HRs showed negative tendencies for OH and O3 levels, the effects of HR(HO2) on the tropospheric abundance of O3 showed a small increment with an increasing loss rate. However, this positive tendency turns to reduction at higher rates (>5 times). Our results demonstrate that the HRs affect not only polluted areas but also remote areas such as the mid-latitude sea boundary layer and upper troposphere. Furthermore, HR(HO2) can bring challenges to pollution reduction efforts because it causes opposite effects between NOx (increase) and surface O3 (decrease). [ABSTRACT FROM AUTHOR]

A long-term, robust observational record of atmospheric black carbon (BC) concentrations at Fukue Island for 2009–2019 was produced by unifying data from a continuous soot-monitoring system and a multi-angle absorption photometer. This record was then used to analyze emission trends from China. We identified a rapid reduction in BC concentrations of (−5.8 ± 1.5) % y−1 or −48 % from 2010 to 2018. We concluded that an emission change of (−5.3 ± 0.7) % y−1, related to changes in China of as much as −4.6 % y−1, was the main underlying driver. This evaluation was made after correcting for the interannual meteorological variability, by using regional atmospheric chemistry model simulations (WRF/CMAQ) with constant emissions. This resolves current fundamental disagreements about the sign of the BC emission trend from China over the past decade, assessed from bottom-up emission inventories; our analysis supported inventories reflecting the governmental clean air actions after 2010 (e.g., MEIC1.3, ECLIPSE v5a and v6b, and REAS updated) and recommended revision to those not (e.g., CEDS). Our estimated emission trends were fairly uniform over seasons but diverse among air-mass origins. Stronger BC reductions occurred in regions of South-Central East China, accompanied by CO emission reduction, while weaker BC reductions occurred in North-Central East China and Northeast China. Prior to 2017, the BC and CO emission trends were both unexpectedly positive in Northeast China during winter months, possibly influencing climate at higher latitudes. The pace of emission reduction over China surpasses those of SSP1 scenarios (SSP: shared socioeconomic pathways) for 2015–2030, suggesting highly successful emission control policies. At Fukue Island, the BC fraction of PM2.5 also steadily decreased over the last decade, suggesting that BC emission reduction started without significant delay with respect to other pollutants, such as NOx and SO2, which are among key precursors of scattering PM2.5. [ABSTRACT FROM AUTHOR]

The Arctic environment is undergoing rapid changes such as faster warming than the global average and exceptional melting of glaciers in Greenland. Black carbon (BC) particles, which are a short-lived climate pollutant, are one cause of Arctic warming and glacier melting. However, the sources of BC particles are still uncertain. We simulated the potential emission sensitivity of atmospheric BC present over the Arctic (north of 66° N) using the Flexpart Lagrangian transport model (version 10.1). This version includes a new aerosol wet removal scheme, which better represents particle-scavenging processes than older versions did. Arctic BC at the surface (0–500 m) and high altitudes (4750–5250 m) is sensitive to emissions in high latitude (> 60° N) and mid-latitude (30–60° N) regions, respectively. Geospatial sources of Arctic BC were quantified, with a focus on emissions from anthropogenic activities and biomass burning in 2010. We found that anthropogenic sources contributed 82 % and 83 % of annual Arctic BC at the surface and high altitudes, respectively. Arctic surface BC comes predominantly from anthropogenic emissions in Russia (56 %), with gas flaring from the Yamalo-Nenets Autonomous Okrug and Komi Republic being the main source (31 % of Arctic surface BC). These results highlight the need for regulations to control BC emissions from gas flaring to mitigate the rapid changes in the Arctic environment. In summer, combined biomass burning in Siberia, Alaska, and Canada contributes 56–85 % (75 % on average) and 40–72 % (57 %) of Arctic BC at the surface and high altitudes, respectively. A large fraction (40 %) of BC in the Arctic at high altitudes comes from anthropogenic emissions in East Asia, which suggests that the rapidly growing economies of developing countries could have a non-negligible effect on the Arctic. To our knowledge, this is the first year-round evaluation of Arctic BC sources that has been performed using the new wet deposition scheme in Flexpart. The study provides a scientific basis for actions to mitigate the rapidly changing Arctic environment. [ABSTRACT FROM AUTHOR]

Constraints from ozone (O3) observations over oceans are needed in addition to those from terrestrial regions to fully understand global tropospheric chemistry and its impact on the climate. Here, we provide a large data set of ozone and carbon monoxide (CO) levels observed (for 11666 and 10681h, respectively) over oceans. The data set is derived from observations made during 24 research cruise legs of R/V Mirai during 2012 to 2017, in the Southern, Indian, Pacific, and Arctic Oceans, covering the region from 67°S to 75°N. The data are suitable for critical evaluation of the over-ocean distribution of ozone derived from chemical transport models. We first give an overview of the statistics in the data set and highlight key features in terms of geographical distribution and air mass type. We then use the data set to evaluate ozone concentration fields from Tropospheric Chemistry Reanalysis version 2 (TCR-2), produced by assimilating a suite of satellite observations of multiple species into a chemical transport model, namely CHASER. For long-range transport of polluted air masses from continents to the oceans, during which the effects of forest fires and fossil fuel combustion were recognized, TCR-2 gave an excellent performance in reproducing the observed temporal variations and photochemical buildup of O3 when assessed from ΔO3/ΔCO ratios. For clean marine conditions with low and stable CO concentrations, two focused analyses were performed. The first was in the Arctic (>70°N) in September every year from 2013 to 2016; TCR-2 underpredicted O3 levels by 6.7ppb (21%) on average. The observed vertical profiles from O3 soundings from R/V Mirai during September 2014 had less steep vertical gradients at low altitudes (>850hPa) than those obtained TCR-2. This suggests the possibilities of more efficient descent of the O3-rich air from above or less efficient dry deposition on the surface than were assumed in the model. In the second analysis, over the western Pacific equatorial region (125-165°E, 10°S to 25°N), the observed O3 level frequently decreased to less than 10ppb in comparison to that obtained with TCR-2, and also those obtained in most of the Atmospheric Chemistry Climate Model Intercomparison Project (ACCMIP) model runs for the decade from 2000. These results imply loss processes that are unaccounted for in the models. We found that the model's positive bias positively correlated with the daytime residence times of air masses over a particular grid, namely 165-180°E and 15-30°N; an additional loss rate of 0.25ppbh-1 in the grid best explained the gap. Halogen chemistry, which is commonly omitted from currently used models, might be active in this region and could have contributed to additional losses. Our open data set covering wide ocean regions is complementary to the Tropospheric Ozone Assessment Report data set, which basically comprises ground-based observations, and enables a fully global study of the behavior of O3. [ABSTRACT FROM AUTHOR]

The emission characteristics of refractory black carbon (rBC) from biomass burning are essential information for numerical simulations of regional pollution and climate effects. We conducted combustion experiments in the laboratory to investigate the emission ratio and mixing state of rBC from the burning of wheat straw and rapeseed plants, which are the main crops cultivated in the Yangtze River Delta region of China. A single particle soot photometer (SP2) was used to measure rBC-containing particles at high temporal resolution and with high accuracy. The combustion state of each burning case was indicated by the modified combustion efficiency (MCE), which is calculated using the integrated enhancement of carbon dioxide and carbon monoxide concentrations relative to their background values. The mass size distribution of the rBC particles showed a lognormal shape with a mode mass equivalent diameter (MED) of 189 nm (ranging from 152 to 215 nm), assuming an rBC density of 1.8 g cm-3. rBC particles less than 80 nm in size (the lower detection limit of the SP2) accounted for ~5% of the total rBC mass, on average. The emission ratios, which are expressed as ΔrBC/ΔCO (1 indicates the difference between the observed and background values), displayed a significant positive correlation with the MCE values and varied between 1.8 and 34 ng m-3 ppbv-1. Multi-peak fitting analysis of the delay time (1t, or the time of occurrence of the scattering peak minus that of the incandescence peak) distribution showed that rBC-containing particles with rBC MED = 200±10 nm displayed two peaks at Δt = 1.7 μs and Δt = 3.2 μs, which could be attributed to the contributions from both flaming and smoldering combustion in each burning case. Both the Δt values and the shell / core ratios of the rBC-containing particles clearly increased as the MCE decreased from 0.98 (smoldering-dominant combustion) to 0.86 (flaming-dominant combustion), implying the great importance of the rapid condensation of semi-volatile organics. This laboratory study found that the mixing state of rBC particles from biomass burning strongly depends on its combustion processes, and overall MCE should be taken carefully into consideration while the climate effect of rBC particles from open biomass burning is simulated. [ABSTRACT FROM AUTHOR]

We implemented a tagged tracer method of black carbon (BC) into a global chemistry transport model, GEOSChem, examined the pathways and efficiency of long-range transport from a variety of anthropogenic and biomass burning emission sources to the Arctic, and quantified the source contributions of individual emissions. Firstly, we evaluated the simulated BC by comparing it with observations at the Arctic sites and examined the sensitivity of an aging parameterization and wet scavenging rate by ice clouds. For tagging BC, we added BC tracers distinguished by source types (anthropogenic and biomass burning) and regions; the global domain was divided into 16 and 27 regions for anthropogenic and biomass burning emissions, respectively. Our simulations showed that BC emitted from Europe and Russia was transported to the Arctic mainly in the lower troposphere during winter and spring. In particular, BC transported from Russia was widely spread over the Arctic in winter and spring, leading to a dominant contribution of 62% to the Arctic BC near the surface as the annual mean. In contrast, BC emitted from East Asia was found to be transported in the middle troposphere into the Arctic mainly over the Sea of Okhotsk and eastern Siberia during winter and spring. We identified an important "window" area, which allowed a strong incoming of East Asian BC to the Arctic (130- 180° E and 3-8 km of altitude at 66° N). The model demonstrated that the contribution from East Asia to the Arctic had a maximum at about 5 km of altitude due to uplifting during long-range transport in early spring. The efficiency of BC transport from East Asia to the Arctic was lower than that from other large source regions such as Europe, Russia, and North America. However, the East Asian contribution was the most important for BC in the middle troposphere (41 %) and the BC burden over the Arctic (27 %) because of the large emissions from this region. These results suggested that the main sources of Arctic BC differed with altitude. The contribution of all the anthropogenic sources to Arctic BC concentrations near the surface was dominant (90 %) on an annual basis. The contributions of biomass burning in boreal regions (Siberia, Alaska, and Canada) to the annual total BC deposition onto the Arctic were estimated to be 12-15 %, which became the maximum during summer. [ABSTRACT FROM AUTHOR]

Ground-based measurements of black carbon (BC) were performed near an industrial source region in the early summer of 2014 and at a remote island in Japan in the spring of 2015. Here, we report the temporal variations in the transport, size distributions, and mixing states of the BC-containing particles. These particles were characterized using a continuous soot monitoring system, a single particle soot photometer, and an aerosol chemical speciation monitor. The effects of aging on the growth of BC-containing particles were examined by comparing the ground-based observations between the near-source and remote island sites. Secondary formation of sulfate and organic aerosols strongly affected the increases in BC coating (i.e., enhancement of cloud condensation nuclei activity) with air mass aging from the source to the outflow regions. The effects of wet removal on BC microphysics were elucidated by classifying the continental outflow air masses depending on the enhancement ratios of BC to CO (ΔBC/ ΔCO), which were used as an indicator of the transport efficiency of BC. It was found that ΔBC/ ΔCO ratios were controlled mainly by the wet removal during transport in the planetary boundary layer (PBL) on the timescale of 1-2 days. The meteorological conditions and backward trajectory analyses suggested that air masses strongly affected by wet removal originated mainly from a region in southern China (20-35° N) in the spring of 2015. Removal of large and thickly coated BC-containing particles was detected in the airmasses that were substantially affected by the wet removal in the PBL, as predicted by Köhler theory. The size and water solubility of BC-containing particles in the PBL can be altered by the wet removal as well as the condensation of non-BC materials. [ABSTRACT FROM AUTHOR]

Long-term (2009-2015) observations of atmospheric black carbon (BC) mass concentrations were performed using a continuous soot-monitoring system (COSMOS) at Fukue Island, western Japan, to provide information on wet removal rate constraints and the emission strengths of important source regions in East Asia (China and others). The annual average mass concentration was 0.36 µg m-3, with distinct seasonality; high concentrations were recorded during autumn, winter, and spring and were caused by Asian continental outflows, which reached Fukue Island in 6-46 h. The observed data were categorized into two classes, i.e., with and without a wet removal effect, using the accumulated precipitation along a backward trajectory (APT) for the last 3 days as an index. Statistical analysis of the observed ΔBC ∕ ΔCO ratios was performed to obtain information on the emission ratios (from data with zero APT only) and wet removal rates (including data with nonzero APTs). The estimated emission ratios (5.2-6.9 ng m-3 ppb-1) varied over the six air mass origin areas; the higher ratios for south-central East China (30-35° N) than for north-central East China (35-40° N) indicated the relative importance of domestic emissions and/or biomass burning sectors. The significantly higher BC ∕ CO emission ratios adopted in the bottom-up Regional Emission inventory in Asia (REAS) version 2 (8.3-23 ng m-3 ppb-1) over central East China and Korea needed to be reduced at least by factors of 1.3 and 2.8 for central East China and Korea, respectively, but the ratio for Japan was reasonable. The wintertime enhancement of the BC emission from China, predicted by REAS2, was verified for air masses from south-central East China but not for those from north-central East China. Wet removal of BC was clearly identified as a decrease in the ΔBC ∕ ΔCO ratio against APT. The transport efficiency (TE), defined as the ratio of the ΔBC ∕ ΔCO ratio with precipitation to that without precipitation, was fitted reasonably well by a stretched exponential decay curve against APT; a single set of fitting parameters was sufficient to represent the results for air masses originating from different areas. An accumulated precipitation of 25.5 ± 6.1 mm reduced the TE to 1∕e. BC-containing particles traveling to Fukue must have already been converted from hydrophobic to hydrophilic particles, because the behavior of TE against APT was similar to that of PM2.5, the major components of which are hydrophilic. Wet loss of BC greatly influenced interannual variations in the ΔBC ∕ ΔCO ratios and BC mass concentrations. This long-term data set will provide a benchmark for testing chemical transport/climate model simulations covering East Asia. [ABSTRACT FROM AUTHOR]

Ground-based measurements of black carbon (BC) were performed near an industrial source region in the early summer of 2014 and at a remote island in Japan in the spring of 2015. We report the temporal variations in the transport, size distributions, and mixing states of the BC-containing particles measured using a continuous soot monitoring system, a single particle soot photometer, and an aerosol chemical speciation monitor. The effects of aging on the growth of BC-containing particles were examined by comparing the ground-based observations between the near-source and remote island sites. Secondary formation of sulfate aerosol through gas-and cloud-phase reactions strongly affected the increases in BC coating (i.e., enhancement of cloud condensation nuclei activity) with air mass aging from the source to the outflow regions. The effects of the wet removal on the BC microphysics were elucidated by classifying the continental outflow air masses depending on the enhancement ratio of BC to CO (ΔBC / ΔCO) ratios as an indicator of the transport efficiency of BC. It was found that ΔBC / ΔCO ratios were controlled mainly by the rainout process during transport in the planetary boundary layer (PBL) on the timescale of 1-2 days. The meteorological conditions and backward trajectory analyses suggested that air masses strongly affected by rainout originated mainly from Southern China region (20º-35º N) during this season. Selective removal of large and thickly-coated BC-containing particles was found in air masses substantially affected by the rainout in the PBL, as predicted by Köhler theory. The size and water-solubility of BC-containing particles in the PBL can be altered by the rainout process as well as the condensation of non-BC materials. [ABSTRACT FROM AUTHOR]

The coating of black carbon (BC) with inorganic salts and organic compounds can enhance the magnitude of light absorption by BC. To elucidate the enhancement of light absorption of aged BC particles and its relation to the mixing state and morphology of individual particles, we conducted observations of particles at an Asian outflow site in Noto Peninsula, Japan, in the spring of 2013. Absorption and scattering coefficients at 405, 532, and 781 nm and mass concentrations/mixing states of refractory BC in PM2.5 were measured using a three-wavelength photoacoustic soot spectrometer and a single-particle soot photometer (SP2), respectively, after passage through a thermodenuder (TD) maintained at 300 or 400 °C or a bypass line maintained at room temperature (25 °C). The average enhancement factor of BC light absorption due to coating was estimated by comparing absorption coefficients at 781 nm for particles that with and without passing through the TD at 300 °C and was found to be 1.22. The largest enhancements (> 1.30) were observed under high absorption coefficient periods when the air mass was long-range transported from urban areas in China. Aerosol samples were also analyzed using a transmission electron microscope (TEM) equipped with an energy dispersive Xray analyzer. The morphological features and mixing states of soot-containing particles of four samples collected during the high absorption events were analyzed by comparing microphotographs before and after the evaporation of beamsensitive materials by irradiation with a high-density electron beam. The majority of the soot in all samples was found as mixed particles with sulfate-containing spherules or as clusters of such spherules. For samples showing high enhancement (> 1.30) of BC light absorption, the TEM showed that the internally mixed soot-containing particles tended to have a more spherical shape and to be thickly coated. The SP2 measurements also suggested that the proportion of thickly coated soot was greater. Thus, the observed enhancement of BC light absorption was found to differ according to the mixing states and morphology of soot-containing particles. The enhancement of BC light absorption in our in situ measurements and its relation with individual features of sootcontaining particles will be useful to evaluate direct radiative forcing in the downwind areas of large emission sources of BC. [ABSTRACT FROM AUTHOR]