Source apportionment of anthropogenic and biogenic organic aerosol over the Tokyo metropolitan area from forward and receptor models.

Organic aerosol (OA) is a dominant component of PM2.5, and accurate knowledge of its sources is critical for identification of cost-effective measures to reduce PM2.5. For accurate source apportionment of OA, we conducted field measurements of organic tracers at three sites (one urban, one suburban, and one forest) in the Tokyo Metropolitan Area and numerical simulations of forward and receptor models. We estimated the source contributions of OA by calculating three receptor models (positive matrix factorization, chemical mass balance, and secondary organic aerosol (SOA)-tracer method) using the ambient concentrations, source profiles, and production yields of OA tracers. Sensitivity simulations of the forward model (chemical transport model) for precursor emissions and SOA formation pathways were conducted. Cross-validation between the receptor and forward models demonstrated that biogenic and anthropogenic SOA were better reproduced by the forward model with updated modules for emissions of biogenic volatile organic compounds (VOC) and for SOA formation from biogenic VOC and intermediate-volatility organic compounds than by the default setup. The source contributions estimated by the forward model generally agreed with those of the receptor models for the major OA sources: mobile sources, biomass combustion, biogenic SOA, and anthropogenic SOA. The contributions of anthropogenic SOA, which are the main focus of this study, were estimated by the forward and receptor models to have been between 9 % and 15 % in summer 2019. The observed percent modern carbon data indicate that the amounts of anthropogenic SOA produced during daytime have substantially declined from 2007 to 2019. This trend is consistent with the decreasing trend of anthropogenic VOC, suggesting that reduction of anthropogenic VOC has been effective in reducing anthropogenic SOA in the atmosphere.

Approaches to the source evaluation of chlorinated polycyclic aromatic hydrocarbons in fine particles.

Chlorinated polycyclic aromatic hydrocarbons (ClPAHs) have been recognized as novel hazardous pollutants; however, the dominant sources remain unclear. This study investigates the occurrences of ClPAHs in five stages of size-segregated particles collected from an urban site and evaluates the sources and factors affecting the concentrations using organic and inorganic source tracers. ClPAHs are the most frequently detected in the finest particle fraction (less than 1.1 µm; PM1.1), similar to polycyclic aromatic hydrocarbons (PAHs), hopanes, and levoglucosan (LEV). The concentrations of total ClPAHs in PM1.1 shows a significant correlation (p < 0.05) with those of total PAHs and specific hopanes but not to LEV and biogenic fatty acids; this suggests that ClPAHs dominantly originate from industrial activities and vehicular emissions. Heatmap analysis, including source tracers, is used to categorize the possible sources of ClPAHs into three types: ClPAH-specific sources, local industrial activities and vehicular emissions, and remote industrial activities. Furthermore, correlation network analysis is used to clarify the relationships between the pollutants.

Time-resolved characterization of organic compounds in PM2.5 collected at Oki Island, Japan, affected by transboundary pollution of biomass and non-biomass burning from Northeast China.

To evaluate the transboundary pollution of organic aerosols from Northeast Asia, a highly time-resolved measurement of organic compounds was performed in March 2019 at Oki Island located in Japan, which is a remote site and less affected by local anthropogenic sources. PM2.5, water-soluble organic carbon (WSOC) concentrations, and WSOC fraction in PM2.5 showed high values on March 22-23 (high-WSOC period (HWSOC)) when the air mass passed through the area where many fire spots were detected in Northeast China. Biomass burning tracers showed higher concentration, especially levoglucosan exceeded 1 µg/m3 during the HWSOC than the low-WSOC period (LWSOC). Notably, high time-resolved measurements of biomass burning tracers and back trajectory analysis during HWSOC revealed a difference in the variation of lignin pyrolyzed compounds and anhydrous sugars on 22 and 23 March. The air mass passed to different areas in Northeast China in which fire spots were detected, such as the eastern area on the 22nd and the western area on the 23rd. Almost-organic compounds also showed high concentration and strong correlations with levoglucosan and sulfate during HWSOC. Moreover, low-carbon dicarboxylic acids (e.g., adipic acid) and secondary products from anthropogenic volatile organic compounds (e.g., 2,3-dihydroxy-4-oxopentanoic, phthalic, 5-nitrosalicylic acids), also showed a strong correlation with sulfate ions during the HWSOC and LWSOC, respectively. These higher concentrations and strong correlations with levoglucosan and sulfate during the HWSOC propose that their generation could be enhanced by biomass burning. The ratios of organics (e.g., levoglucosan/mannnosan, pinic/3-methylbutane-1,2,3-tricarboxylic acids) suggest that the high concentrations of PM2.5 and WSOC observed during the HWSOC were caused by aged organic aerosols that originated from the combustion of herbaceous plants transported from Northeast China. Our findings indicate that biomass combustion in Northeast China could significantly affect the chemical compositions and the characterization of organic aerosols in downwind regions of Northeast China.

A twenty-year deposition record of elemental carbon in Northern Japan retrieved from archived filters.

The black carbon or elemental carbon (EC) content in ice and snow has been a concern in climate change studies, but time-series records have mostly been obtained from glacier ice-core samples in limited geographical locations, such as the Arctic or high mountains. This is the first study to present decade-long records of EC deposition measured at urban (Sapporo) and background (Rishiri Island) sites in Japan, in the mid-latitude zone of the eastern edge of the Asian continent. By using archived membrane filters from an acid rain study, we retrieved monthly EC deposition records of 1993-2012 in Sapporo and intermittent deposition data in Rishiri. Annual EC deposition showed large fluctuations, with a maximum in 2000-2001 and a minor increase in 2010-2011. This interannual change was moderately related to the deposition of non-sea salt SO42- and the collected water volume but did not reflect the estimated emission history of China. High depositions in 2000-2001 were probably caused by the transport of Asian Dust accompanied by air pollutants, which were characteristically active in these years. The findings of this study have implications for the use of observational data in validating global aerosol transport models.

Health effects of PM2.5 sources on children's allergic and respiratory symptoms in Fukuoka, Japan.

Exposure to fine particulate matter (PM2.5) is a potential aggravating factor for respiratory and allergic diseases. However, which PM2.5 sources are associated with such diseases remains unclear. This study aimed to investigate the association of PM2.5 sources with allergic and respiratory symptoms in schoolchildren. PM2.5 samples were collected in Fukuoka during the spring in 2014 and 2015. Asian dust was observed in 2014. Ion components, elemental components, and organic components were analyzed. Positive matrix factorization (PMF) was conducted to calculate PM2.5 concentrations from each source. Mixed logistic regression analysis with a random intercept for each schoolchild was performed to evaluate the association of components and sources with symptoms. Among 2317 schoolchildren, the mean prevalence was 28.9%, 23.6%, 11.2%, and 11.4% for lower respiratory, nasal, ocular, and skin symptoms, respectively. PMF identified the following six PM2.5 sources "Secondary sulfate and coal combustion", "Secondary nitrate", "Heavy oil combustion", "Sea salt", "Soil" and "Traffic emission". An interquartile range of PM2.5 mass was associated with nasal (Odds ratios 1.08, 95% confidence interval [1.03, 1.13]), ocular (1.10, [1.04, 1.16]), and skin symptoms (1.13, [1.06, 1.20]). Among the source factors, "Heavy oil combustion" was significantly associated with nasal symptom (1.11, [1.05, 1.18]) while "Sea salt" was associated with nasal (1.06, [1.02, 1.11]) and skin (1.073, [1.01, 1.14]) symptoms. We found "Soil", which might be affected by Asian dust, was associated with ocular (1.07, [1.03, 1.10]) and skin (1.05, [1.01, 1.08]) symptoms. Further studies in other seasons or places are needed to clarify the influence of PM2.5 sources on children's health.

Evaluation of the genotoxicity of PM2.5 collected by a high-volume air sampler with impactor.

BACKGROUND: The harmful effects of fine particles with an aerodynamic diameter less than 2.5 µm (PM2.5) on respiratory organs are emphasized in pollution studies because PM2.5 have high deposition rates in the respiratory organs and contain various hazardous compounds. In this study, a sampling method combining a high-volume air sampler (HV) with a PM2.5 impactor was developed for collecting large quantities of PM2.5. The concentrations of elemental carbon (EC), organic carbon (OC), inorganic ions, and polycyclic aromatic hydrocarbons (PAHs) were measured in PM2.5 collected by the high-and low-volume air samplers (LV). RESULTS: Similar results were obtained from the HV and LV methods, with respect to inorganic carbon, organic carbon, sodium ions, ammonium ions, and PAHs with more than four rings. Because of the much larger amount of PM2.5 could be collected by the HV method, the trace constituents, that were difficult to detect by the conventional LV method, were readily detected by the HV method. Furthermore, when the microsuspension method that was modified more sensitive Ames mutagenicity test, was used to test the PM2.5 samples at four sites, mutagenic activities were detected by strains TA100 and TA98. Most of the mutagenic activity was associated with the PM2.5 fraction and mutagenic activity in winter was greater than that in summer. CONCLUSIONS: The HV method produced results similar to those from the conventional LV method with respect to the PM2.5 components present in the atmosphere in relatively high concentrations, but its 40-fold greater flow rate enabled the detection of mutagenic compounds present in only trace concentrations.

The influence of the open burning of agricultural biomass and forest fires in Thailand on the carbonaceous components in size-fractionated particles.

Size-segregated ambient particles down to particles smaller than 0.1 µm (PM0.1) were collected during the year 2014-2015 using cascade air samplers with a PM0.1 stage, at two cities in Thailand, Bangkok and Chiang Mai. Their characteristics and seasonal behavior were evaluated based on the thermal/optical reflectance (IMPROVE_TOR) method. Diagnostic indices for their emission sources and the black carbon (BC) concentration were assessed using an aethalometer and related to the monthly emission inventory (EI) of particle-bound BC and organic carbon (OC) in order to investigate the contribution of agricultural activities and forest fires as well as agro-industries in Thailand. Monthly provincial EIs were evaluated based on the number of agricultural crops produced corresponding to field residue burning and the use of residues as fuel in agro-industries, and also on the number of hot spots from satellite images corresponding to the areas burned by forest fires. The ratio of char-EC/soot-EC describing the relative influence of biomass combustion to diesel emission was found to be in agreement with the EI of BC from biomass burning in the size range <1 µm. This was especially true for PM0.1, which usually tends to be indicative of diesel exhaust particles, and was shown to be very sensitive to the EI of biomass burning. In Chiang Mai, the northern part of Thailand, the forest fires located upwind of the monitoring site were found to be the largest contributor while the carbon behavior at the site in Bangkok was better accounted for by the EI of provinces in central Thailand including Bangkok and its surrounding provinces, where the burning of crop residues and the cultivation of sugarcane for sugar production are significant factors. This suggests that the influence of transportation of polluted air masses is important on a multi-provincial scale (100-200 km) in Thailand.

Distributions and multiple sources of chlorinated polycyclic aromatic hydrocarbons in the air over Japan.

Chlorinated polycyclic aromatic hydrocarbons (ClPAHs) have been detected in the air at discrete sites in Japan, but there is no information on their distributions throughout Japan. This study was a widespread survey of atmospheric concentrations of ClPAHs throughout Japan. The majority of 24 species of ClPAHs were detected in either the gas or particle phase at all sampling sites. The concentrations were weakly related to human population densities. The relationships between total concentrations of ClPAHs and PAHs suggested that atmospheric ClPAHs at ~70% of the sites were derived from common sources of PAHs. A ternary diagram based on diagnostic ratios of 1-chloropyrene, 7-chlorobenz[a]anthracene, and 6-chlorobenzo[a]pyrene normalized to 3-chlorofluoranthene suggested that waste combustion was the likely source of ClPAHs in summer and that vehicular emissions and coal burning were the likely sources of ClPAHs in winter. A heat map analysis estimated from the concentrations of individual compounds at each site suggested that there were three categories of sources at the sites: i) common sources of ClPAHs and PAHs that had moderate impacts, ii) common sources of ClPAHs and PAHs that had high impacts, and iii) specific sources of ClPAHs.

Impact of field biomass burning on local pollution and long-range transport of PM2.5 in Northeast Asia.

Biomass burning (BB), such as, crop field burning during the post-harvest season, emits large amounts of air pollutants (e.g., PM2.5) that severely impact human health. However, it is challenging to evaluate the impact of BB on PM2.5 due to uncertainties in the size and location of sources as well as their temporal and spatial variability. This study focused on the impacts of BB on local pollution as well as the long-range transport of PM2.5 in Northeast Asia resulting from a huge field BB event in Northeast China during the autumn of 2014. Air quality simulations using the Community Multiscale Air Quality (CMAQ) model were conducted in the year 2014 over the horizontal domains covering Northeast Asia, including the Japanese mainland. In the baseline simulation (Base), field BB emissions were derived from Fire INventory from NCAR (FINN) v1.5 for the year 2014. The model reasonably captured the daily mean PM2.5 mass concentrations, however, it underestimated concentrations in autumn around Northeast China where irregular field BB following the harvest occurred frequently. To address the underestimation of emissions from BB sources in China, another simulation with boosted BB sources from cropland area (FINN20_crop) was conducted in addition to the Base simulation. The model performance of FINN20_crop was significantly improved and showed smaller biases and higher indices of agreement between simulated and observed values in comparison to those of Base. To evaluate long-range transport of PM2.5 from BB sources in China towards Japan, CMAQ with brute-force method (CMAQ/BFM)-estimated BB contributions for Base and FINN20_crop cases were compared with Positive Matrix Factorization (PMF)-estimated BB contributions at Noto Peninsula in Japan. The CMAQ/BFM-estimated contributions from FINN20_crop were in greater agreement with the PMF-estimated contributions. The comparison of BB contributions estimated by the two contrasting models also indicated large underestimations in the current BB emission estimates.

Structural and Light-Absorption Characteristics of Complex Water-Insoluble Organic Mixtures in Urban Submicrometer Aerosols.

Submicrometer aerosols in the urban atmosphere of Nagoya, Japan, were collected in late winter and early spring, and the water-insoluble organic matter (WISOM) in the samples were fractionated into six subfractions based on their polarities by using solvent and normal-phase solid-phase extractions: nonpolar (F1), low-polar (F2 and F3), and medium-polar (F4, F5, and F6) fractions. The overall structural characteristics of these subfractions were then analyzed using Fourier transform infrared spectroscopy, nuclear magnetic resonance spectroscopy, and high-resolution aerosol mass spectrometry. Quantitative information related to the overall chemical characteristics of the WISOM in the different polarity fractions, including their elemental compositions, the relative abundances of different functional groups and their fragments from electron impact ionization, was obtained. These water-insoluble fractions accounted for half of the total light absorption by the extracted aerosol matter at 400 nm. The contributions of the medium-polar fractions to both the total organic carbon and light absorption by the extracts were dominant among the contributions from the six subfractions. Large molecules with aromatic and heteroatomic (O and N) groups, including charge transfer complexes, might have greatly contributed to the light absorption by the fraction F4, which is the largest fraction of the extracted water-insoluble organic matter.

Weak size dependence of resuspended radiocesium adsorbed on soil particles collected after the Fukushima nuclear accident.

Most studies of the properties of airborne radionuclides emitted from the Fukushima Daiichi Nuclear Power Plant have focused on the relatively early stages of the accident, and little is known about the characteristics of radiocesium in the long-term. In this study, we analyzed activity size distributions of airborne radiocesium collected over 5 months in Tsukuba, Japan. Radiocesium in the accumulation mode size range (0.1-2 µm in aerodynamic diameter) was overwhelming in the early aerosol samples and decreased with time, while that associated with coarse aerosols remained airborne. We examined the radiocesium adsorbed onto airborne soil particles, and found that the size dependence of 137Cs surface density adsorbed on soil particles was weak. That is, radiocesium was distributed homogeneously throughout the aerodynamic diameter range of 2.1-11 µm. This characteristic may be related to the reported structure of radiocesium-bearing soil particles collected from the ground, which consisted of an aggregate of specific clay minerals and other non-cesium adsorbing particles. The resuspension factors for the first two aerosol samples collected during late April and May 2011 were close to those in European cities in the months following the Chernobyl accident, despite different soil and weather conditions.

Source apportionment of chlorinated polycyclic aromatic hydrocarbons associated with ambient particles in a Japanese megacity.

Chlorinated polycyclic aromatic hydrocarbons (ClPAHs) are novel species of environmental contaminants whose possible sources remain unclear. The occurrence of ClPAHs within total suspended particles (TSP) is compared with weekly air samples at two sites of differing characteristics (industrial and residential) in the megacity of Nagoya, Japan. Samples were collected over 12 months during 2011-2012. All 24 species of targeted ClPAHs were detected at both industrial and residential sites, where mean concentrations of total ClPAHs in TSP were 20.7 and 14.1 pg/m3, respectively. High concentrations at the industrial site were frequently observed during winter, suggesting potent seasonal ClPAH sources there. Positive matrix factorization modeling of particulate ClPAH source identification and apportioning were conducted for datasets including ClPAHs, PAHs, elements and ions, plus elemental carbons in TSP. Eight factors were identified as possible ClPAH sources, with estimates that the dominant one was a specific source of ClPAH emission (31%), followed by traffic (23%), photodegradable and semi-volatile species (18%), long-range transport (11%), and industry and oil combustion (10%). Source contributions of ClPAHs differed substantially from those of PAHs. This suggests specific and/or potent ClPAH sources in the local area, and that the production mechanisms between ClPAHs and PAHs are substantially different.

Light Absorption and Excitation-Emission Fluorescence of Urban Organic Aerosol Components and Their Relationship to Chemical Structure.

The present study used a combination of solvent and solid-phase extractions to fractionate organic compounds with different polarities from total suspended particulates in Nagoya, Japan, and their optical characteristics were obtained on the basis of their UV-visible absorption spectra and excitation-emission matrices (EEMs). The relationship between their optical characteristics and chemical structures was investigated based on high-resolution aerosol mass spectra (HR-AMS spectra), soft ionization mass spectra and Fourier transform infrared (FT-IR) spectra. The major light-absorption organics were less polar organic fractions, which tended to have higher mass absorption efficiencies (MAEs) and lower wavelength dependent Ångström exponents (Å) than the more polar organic fractions. Correlation analyses indicate that organic compounds with O and N atoms may contribute largely to the total light absorption and fluorescence of the organic aerosol components. The extracts from the aerosol samples were further characterized by a classification of the EEM profiles using a PARAFAC model. Different fluorescence components in the aerosol organic EEMs were associated with specific AMS ions and with different functional groups from the FT-IR analysis. These results may be useful to determine and further classify the chromophores in atmospheric organic aerosols using EEM spectroscopy.

Local and seasonal variations in concentrations of chlorinated polycyclic aromatic hydrocarbons associated with particles in a Japanese megacity.

Concentrations of particle-bound polycyclic aromatic hydrocarbons (PAHs) and chlorinated PAHs (ClPAHs) were measured in different seasons at five sampling stations in Nagoya, a Japanese megacity. The annual mean total ClPAH and total PAH concentrations were 43.3-92.6pg/m(3) and 5200-8570pg/m(3), respectively. The concentrations of total ClPAHs were significantly variable than those of total PAHs, and both total concentrations through the seasons did not significantly correlate at any of the stations. Principal component analysis was used to characterize the ClPAH sources, resulted that ClPAHs were found to be associated with the sources of high-molecular-weight PAHs in the warmer seasons and of low-molecular-weight PAHs in the colder seasons. These findings suggest that principal sources of particle-bound ClPAHs are present in the local area, and change in the seasons. Toxic equivalent (TEQ) concentrations were estimated to assess the risks associated with exposure to ClPAHs in air. The TEQ concentrations in the samples were 0.05-0.32pg-TEQ/m(3). The TEQ concentrations in summer were approximately half the TEQ concentrations in the other seasons at all of the stations.

Comparison of Air Pollution in Metropolises in China (Beijing) and Japan (Osaka and Nagoya) on the Basis of the Levels of Contaminants and Mutagenicity.

Public concern regarding the transport of air pollutants from mainland East Asia to the leeward area by the prevailing westerlies in spring and winter monsoon has been growing in recent years. We collected total suspended particle (TSP) in Beijing, a metropolis of China located windward of Japan, in spring (late February 2011-May 2011) and in winter (November 2012-early February 2013), then analyzed metals, ions, and organic compounds and mutagenicity, and compared the pollution levels with samples collected at two Japanese metropolises (Osaka and Nagoya) during the same periods. The medians of concentration of TSP and other factors in Beijing were much larger than those in the Japanese metropolises. Especially, the concentrations of polycyclic aromatic hydrocarbons (PAHs) were remarkably high in Beijing in winter, and the median of total PAHs concentration in Beijing was 62-63 times larger than that in the Japanese sites. The mutagenicity of TSP from Beijing toward Salmonella typhimurium YG1024, with and without a mammalian metabolic system (S9 mix), was 13-25 times higher than that from the Japanese sites in winter. These results suggest that air pollution levels in Beijing are very high compared with those at the two Japanese metropolises we evaluated. The diagnostic ratios of PAHs and nitrated polycyclic aromatic hydrocarbons (NPAHs) suggest that the major sources of PAHs and NPAHs in Beijing are different from those at the two Japanese sites in winter, and that the major source in Beijing is coal/biomass combustion.

Spatial correlativity of atmospheric particulate components simultaneously collected in Japan.

The simultaneous sampling of total suspended particles was performed at 14 sites in Japan during July 2008-June 2009. The spatial correlativity of each particulate composition toward Osaka was obtained for nine selected sites to overview the chemical composition and geographical distribution of particulate components across a wide range of areas nationwide. The spatial correlatives of atmospheric particulate components were extended to an even wider range of areas up to 950 km distance (meso-alpha scale region, >200 km) for a far-reaching distance analysis unique in the literature. Overall, the spatial correlations of ionic species and both organic and elemental carbons were significant, suggesting their shared advections, including their long-range transport from East Asia. Although sulfate ions are widely dispersed across Japan, such is not necessarily correlated with organic and elemental carbon, possibly indicating that the sulfate emission source, including long-range transport, differs from that of carbonaceous particulates. By contrast, the characteristics of spatial correlatives of metallic constituents vary; for example, particulate Pb and Cd show a significantly wide range of spatial correlatives to Osaka, while Mn-though limited to cities neighboring Osaka-shows significant spatial correlations. Other metallic constituents showed no significant spatial correlatives, indicating the effects of local pollutants. Moreover, the extent of the spatial dispersion of the particulate components and the relationships among chemical components were analyzed via factor analysis to highlight the effects of long-range inflow and local original emissions. In this treatment, 13 particulate components among the 19 measured were implicated in long-range transport.

Chemical Structural Characteristics of HULIS and Other Fractionated Organic Matter in Urban Aerosols: Results from Mass Spectral and FT-IR Analysis.

The chemical characteristics of complex organic matter in atmospheric aerosols remain poorly understood. Water-insoluble organic matter (WISOM) and water-soluble organic matter (WSOM) in the total suspended particulates collected in the city of Nagoya in summer/early autumn and winter were extracted using multiple solvents. Two fractions of humic-like substances, showing neutral and acidic behavior (HULIS-n and HULIS-a, respectively), and the remaining highly polar part (HP-WSOM) were fractionated from WSOM using solid phase extraction. The chemical structural characteristics and concentrations of the organic matter were investigated using mass spectrometry and Fourier transform infrared (FT-IR) spectroscopy. WISOM and HULIS-n had low O/C ratios (0.1 and 0.4, respectively) and accounted for a large fraction of the organics in aerosols (70%). HULIS-a and HP-WSOM had higher O/C ratios (0.7 and 1.0, respectively), and their concentrations in summer and early autumn were on average ∼2 times higher than those in winter. The mass spectrum and FT-IR analyses suggest the following: (1) WISOM were high-molecular-weight aliphatics (primarily C27-C32) with small proportions of -CH3, -OH, and C═O groups; (2) HULIS-n was abundant in aliphatic structures and hydroxyl groups (primarily C9-C18) and by branched structures; (3) HULIS-a and HP-WSOM contained relatively large amounts of low-molecular-weight carboxylic acids and alcohols (primarily C4-C10); and (4) WISOM and HULIS-n were relatively abundant in amines and organic nitrates.

Associations Between Fine Particulate Matter Components and Daily Mortality in Nagoya, Japan.

BACKGROUND: Seasonal variation and regional heterogeneity have been observed in the estimated effect of fine particulate matter (PM2.5) mass on mortality. Differences in the chemical compositions of PM2.5 may cause this variation. We investigated the association of the daily concentration of PM2.5 components with mortality in Nagoya, Japan. METHODS: We combined daily mortality counts for all residents aged 65 years and older with concentration data for PM2.5 mass and components in Nagoya from April 2003 to December 2007. A time-stratified case-crossover design was used to examine the association of daily mortality with PM2.5 mass and each component (chloride, nitrate, sulfate, sodium, potassium, calcium, magnesium, ammonium, elemental carbon [EC], and organic carbon [OC]). RESULTS: We found a stronger association between mortality and PM2.5 mass in transitional seasons. In analysis for each PM2.5 component, sulfate, nitrate, chloride, ammonium, potassium, EC, and OC were significantly associated with mortality in a single-pollutant model. In a multi-pollutant model, an interquartile range increase in the concentration of sulfate was marginally associated with an increase in all-cause mortality of 2.1% (95% confidence interval, -0.1 to 4.4). CONCLUSIONS: These findings suggest that some specific PM components have a more hazardous effect than others and contribute to seasonal variation in the health effects of PM2.5.

Influence of contemporary carbon originating from the 2003 Siberian forest fire on organic carbon in PM2.5 in Nagoya, Japan.

In May 2003, high concentrations of organic carbon (OC) in PM2.5 were measured in Nagoya, a representative metropolitan area in Japan. To investigate the influence of possible forest fires on PM2.5 in Japan via long-range aerosol transport, the radiocarbon ((14)C) concentrations of PM2.5 samples from April 2003 to March 2004 were measured. (14)C concentrations in total carbon (TC) from May to early June showed higher values than those in other periods. The OC/elemental carbon (EC) ratios from May to early June were also significantly higher than the ones in other periods. In addition, OC concentrations from May to early June were typically high. These results indicate that the abundant OC fraction from May to early June in Nagoya consisted predominantly of contemporary carbon. Furthermore, simulations of diffusion and transport of organic matter (OM) in East Asia showed that abundant OM originating from East Siberia spread over East Asia and Japan in May and early June. Backward air mass trajectories from this time frame indicate that the air mass in Nagoya likely first passed through East Siberia where fire events were prevalent. However, the backward trajectories showed that the air mass after early June did not originate mainly from Siberia, and correspondingly, the (14)C and OC concentrations showed lower values than those from May to early June. Therefore, the authors conclude that contemporary carbon originating from the forest fire in East Siberia was transported to Nagoya, where it significantly contributed to the high observed concentrations of both OC and (14)C.

Sulfate aerosol as a potential transport medium of radiocesium from the Fukushima nuclear accident.

To date, areas contaminated by radionuclides discharged from the Fukushima Dai-ichi nuclear power plant accident have been mapped in detail. However, size of the radionuclides and their mixing state with other aerosol components, which are critical in their removal from the atmosphere, have not yet been revealed. We measured activity size distributions of (134)Cs and (137)Cs in aerosols collected 47 days after the accident at Tsukuba, Japan, and found that the activity median aerodynamic diameters of (134)Cs and (137)Cs in the first sample (April 28-May 12) were 0.54 and 0.53 µm, respectively, and those in the second sample (May 12-26) were both 0.63 µm. The activity size distributions of these radiocesium were within the accumulation mode size range and almost overlapped with the mass size distribution of non-sea-salt sulfate aerosol. From the analysis of other aerosol components, we found that sulfate was the potential transport medium for these radionuclides, and resuspended soil particles that attached radionuclides were not the major airborne radioactive substances at the time of measurement. This explains the relatively similar activity sizes of radiocesium measured at various sites during the Chernobyl accident. Our results can serve as basic data for modeling the transport/deposition of radionuclides.