Impacts on air dose rates after the Fukushima accident over the North Pacific from 19 March 2011 to 2 September 2015.

A fleet of thirteen in-service global container ships continuously measured the air dose rates over the North Pacific after the Fukushima Daiichi Nuclear Power Station (FDNPS) accident. The results showed that the elevated air dose rates over the Port of Tokyo and the FDNPS emissions are significantly correlated (log(emission fluxes) = 54.98 x (air dose rates) (R = 0.95, P-value<0.01), and they are also significantly correlated with the Tsukuba deposition fluxes (log(deposition fluxes) = 0.47 + 30.98 (air dose rates) (R = 0.91, P-value<0.01). These results demonstrate the direct impact of the FDNPS emissions on the depositions of radionuclides and the air dose rates over the Port of Tokyo. Over the North Pacific, the correlation equations are log(emission fluxes) = -2.72 + 202.36 x (air dose rates over the northwestern Pacific) (R = 0.40, P-value<0.01), and log(emission fluxes) = -0.55 + 80.19 x (air dose rates over the northeastern Pacific) (R = 0.29, P-value = 0.0424). These results indicate that the resuspension of the deposited radionuclides have become a dominant source in the transport of radionuclides across the North Pacific. Model simulations show underestimated air dose rates during the periods of 22-25 March 2011 and 27-30 March 2011 indicating the lack of mechanisms, such as the resuspension of radionuclides, in the model.

Temporal change of 236U/238U and 235U/238U isotopic ratios in atmospheric deposition in Tokyo and Akita from 1963 to 1979.

We examine the temporal changes of 236U/238U and 235U/238U in atmospheric deposition from samples collected in Tokyo and Akita from 1963 to 1979 and elucidate the spatial distribution and historical changes of the anthropogenic sources of uranium in Japan. The 236U/238U ratio of atmospheric deposition in Tokyo peaked in 1963 and again during the 1970s, while the corresponding 235U/238U ratios of atmospheric deposition during the second peak period were lower than that of natural uranium. The 236U/238U ratios of atmospheric deposition in Akita samples peaked in 1963. The 235U/238U ratios in Akita samples were almost identical to that of the natural uranium ratios. These results suggest that the peak of 236U/238U in 1963 corresponds to what is recognized as representative for global fallout. The increase of 236U/238U and the decrease of 235U/238U observed simultaneously in the 1970s indicate that depleted uranium has subsequently been released into the environment around Tokyo. The cumulative deposition density of 236U for atmospheric fallout samples collected in Tokyo from 1968 to 1979 is an order of magnitude larger than that of the global fallout, suggesting that the depleted uranium in the 1970s is a major component of 236U in Tokyo and should be considered as an end-member when using 236U as an environmental tracer in the industrial city. This knowledge can facilitate future research using 236U as an effective environmental tracer.

Simulation of the transition metal-based cumulative oxidative potential in East Asia and its emission sources in Japan.

The aerosol oxidative potential (OP) is considered to better represent the acute health hazards of aerosols than the mass concentration of fine particulate matter (PM2.5). The proposed major contributors to OP are water soluble transition metals and organic compounds, but the relative magnitudes of these compounds to the total OP are not yet fully understood. In this study, as the first step toward the numerical prediction of OP, the cumulative OP (OPtm*) based on the top five key transition metals, namely, Cu, Mn, Fe, V, and Ni, was defined. The solubilities of metals were assumed constant over time and space based on measurements. Then, the feasibility of its prediction was verified by comparing OPtm* values based on simulated metals to that based on observed metals in East Asia. PM2.5 typically consists of primary and secondary species, while OPtm* only represents primary species. This disparity caused differences in the domestic contributions of PM2.5 and OPtm*, especially in large cities in western Japan. The annual mean domestic contributions of PM2.5 were 40%, while those of OPtm* ranged from 50 to 55%. Sector contributions to the OPtm* emissions in Japan were also assessed. The main important sectors were the road brake and iron-steel industry sectors, followed by power plants, road exhaust, and railways.

Temporal variations of 90Sr and 137Cs in atmospheric depositions after the Fukushima Daiichi Nuclear Power Plant accident with long-term observations.

We have measured artificial radionuclides, such as 90Sr and 137Cs, in atmospheric depositions since 1957 in Japan. We observed the variations in 90Sr and 137Cs, which were emitted from atmospheric nuclear tests and nuclear power plant accidents, due to their diffusion, deposition, and resuspension. In March 2011, the Fukushima Daiichi Nuclear Power Plant accident occurred in Japan, and significant increases in 90Sr and 137Cs were detected at our main site in Tsukuba, Ibaraki. Our continual observations revealed that the 137Cs monthly deposition rate in 2018 declined to ~ 1/8100 of the peak level, but it remained more than ~ 400 times higher than that before the accident. Chemical analysis suggested that dust particles were the major carriers of 90Sr and 137Cs during the resuspension period at our main site. Presently, the effective half-life for 137Cs deposition due to radioactive decay and other environmental factors is 4.7 years. The estimation suggests that approximately 42 years from 2011 are required to reduce the atmospheric 137Cs deposition to a state similar to that before the accident. The current 90Sr deposition, on the other hand, shows the preaccident seasonal variation, and it has returned to the same radioactive level as that before the accident.

Modeling Transition Metals in East Asia and Japan and Its Emission Sources.

Emission inventories of anthropogenic transition metals, which contribute to aerosol oxidative potential (OP), in Asia (Δx = 0.25°, monthly, 2000-2008) and Japan (Δx = 2 km, hourly, mainly 2012) were developed, based on bottom-up inventories of particulate matters and metal profiles in a speciation database for particulate matters. The new inventories are named Transition Metal Inventory (TMI)-Asia v1.0 and TMI-Japan v1.0, respectively. It includes 10 transition metals in PM2.5 and PM10, which contributed to OP based on reagent experiments, namely, Cu, Mn, Co, V, Ni, Pb, Fe, Zn, Cd, and Cr. The contributions of sectors in the transition metals emission in Japan were also investigated. Road brakes and iron-steel industry are primary sources, followed by other metal industry, navigation, incineration, power plants, and railway. In order to validate the emission inventory, eight elements such as Cu, Mn, V, Ni, Pb, Fe, Zn, and Cr in anthropogenic dust and those in mineral dust were simulated over East Asia and Japan with Δx = 30 km and Δx = 5 km domains, respectively, and compared against the nation-wide seasonal observations of PM2.5 elements in Japan and the long-term continuous observations of total suspended particles (TSPs) at Yonago, Japan in 2013. Most of the simulated elements generally agreed with the observations, while Cu and Pb were significantly overestimated. This is the first comprehensive study on the development and evaluation of emission inventory of OP active elements, but further improvement is needed.

Rain-induced bioecological resuspension of radiocaesium in a polluted forest in Japan.

It is the conventional understanding that rain removes aerosols from the atmosphere. However, the question of whether rain plays a role in releasing aerosols to the atmosphere has recently been posed by several researchers. In the present study, we show additional evidence for rain-induced aerosol emissions in a forest environment: the occurrence of radiocaesium-bearing aerosols in a Japanese forest due to rain. We carried out general radioactive aerosol observations in a typical mountainous village area within the exclusion zone in Fukushima Prefecture to determine the impacts and major drivers of the resuspension of radiocaesium originating from the nuclear accident in March 2011. We also conducted sampling according to the weather (with and without rain conditions) in a forest to clarify the sources of atmospheric radiocaesium in the polluted forest. We found that rain induces an increase in radiocaesium in the air in forests. With further investigations, we confirmed that the fungal spore sources of resuspended radiocaesium seemed to differ between rainy weather and nonrainy weather. Larger fungal particles (possibly macroconidia) are emitted during rainy conditions than during nonrainy weather, suggesting that splash generation by rain droplets is the major mechanism of the suspension of radiocaesium-bearing mould-like fungi. The present findings indicate that radiocaesium could be used as a tracer in such research fields as forest ecology, meteorology, climatology, public health and agriculture, in which fungal spores have significance.

Project IPAD, a database to catalogue the analysis of Fukushima Daiichi accident fragmental release material.

The 2011 accident at Japan's Fukushima Daiichi Nuclear Power Plant released a considerable inventory of radioactive material into the local and global environments. While the vast majority of this contamination was in the form of gaseous and aerosol species, of which a large component was distributed out over the neighbouring Pacific Ocean (where it was subsequently deposited), a substantial portion of the radioactive release was in particulate form and was deposited across Fukushima Prefecture. To provide an underpinning understanding of the dynamics of this catastrophic accident, alongside assisting in the off-site remediation and eventual reactor decommissioning activities, the 'International Particle Analysis Database', or 'IPAD', was established to serve as an interactive repository for the continually expanding analysis dataset of the sub-mm ejecta particulate. In addition to a fully interrogatable database of analysis results for registered users (exploiting multiple search methods), the database also comprises an open-access front-end for members of the public to engage with the multi-national analysis activities by exploring a streamlined version of the data.

240Pu/239Pu and 242Pu/239Pu atom ratios of Japanese monthly atmospheric deposition samples during 1963-1966.

Global fallout plutonium isotopic ratios from the 1960s are important for the use of Pu as environmental tracers. We measured the 240Pu/239Pu and 242Pu/239Pu atomic ratios of monthly atmospheric deposition samples collected in Tokyo and Akita, Japan during March 1963 to May 1966. To our knowledge, our results represent the first data measured for actual atmospheric deposition samples collected continuously during the 1960s. Both atomic ratios increased rapidly from March 1963 to June 1963, followed by a gradual increase until September 1963. Then, both ratios declined with a half-life of approximately 5.6 months. The observed temporal changes of the ratios were likely caused by the upper-stratospheric input of nuclear debris from high-yield atmospheric nuclear weapon testing during 1961-62, followed by its downward transport to the troposphere.

A review of Cs-bearing microparticles in the environment emitted by the Fukushima Dai-ichi Nuclear Power Plant accident.

Scientists face challenge in identifying the radioactive materials which are found as dotted images on various imaging plate (IP) autoradiographic photos of radioactively contaminated materials by the Fukushima Dai-ichi Nuclear Power Plant (F1NPP, or FDNPP) accident, such as air filter, fugitive dust, surface soil, agricultural materials, and water-shed samples. It has been revealed that they are minute particles with distinct morphology and elemental composition with high specific radioactivity, and different from those of the so-called Chernobyl hot particles. Basically, they are glassy particles once molten, composed of Si, O, Fe, Zn etc. with highly concentrated radiocaesium, which can be called as radiocaesium-bearing microparticles (CsMP). At present, CsMP can be classified into two types, Types-A and -B, which are characterized by different specific radioactivity, 134Cs/137Cs ratio, size and morphology, and geographic distribution around F1NPP. Such studies on the CsMP from various aspects have provided valuable information about what happened in the nuclear reactors during the F1NPP accident and fates of the CsMP in the environment. This review first provides a retrospective view on the research history of the CsMP, which is helpful to understand the unique character of the CsMP. Subsequently, more details about the current understanding of the natures of these hot particles, such as origin, morphology, chemical compositions, thermal properties, water-solubility, and secondary migration of CsMP in river and ocean systems are described with future prospects.

Fungal spore involvement in the resuspension of radiocaesium in summer.

We observed the atmospheric resuspension of radiocaesium, derived from the Fukushima Dai-ichi Nuclear Power Plant accident, at Namie, a heavily contaminated area of Fukushima, since 2012. During the survey periods from 2012 to 2015, the activity concentrations of radiocaesium in air ranged from approximately 10-5 to 10-2 Bq per m3 and were higher in the warm season than in the cold season. Electron microscopy showed that the particles collected on filters in summer were predominantly of biological origin (bioaerosols), with which the observed radiocaesium activity concentration varied. We conducted an additional aerosol analysis based on fluorescent optical microscopic observation and high-throughput DNA sequencing technique to identify bioaerosols at Namie in 2015 summer. The concentrations of bioaerosols fluctuated the order of 106 particles per m3, and the phyla Basidiomycota and Ascomycota (true Fungi) accounted for approximately two-thirds of the bioaerosols. Moreover, the fungal spore concentration in air was positively correlated with the radiocaesium concentration at Namie in summer 2016. The bioaerosol emissions from Japanese mixed forests in the temperate zone predominately included fungal cells, which are known to accumulate radiocaesium, and should be considered an important scientific issue that must be addressed.

Atmospheric Activity Concentration of 90Sr and 137Cs after the Fukushima Daiichi Nuclear Accident.

On March 11, 2011, the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident occurred and large amounts of radionuclides were discharged into the atmosphere. We have operated continuous aerosol samplings at four locations in Japan from the accident until the end of 2011. The activities of 90Sr and 137Cs in the aerosol samples were measured using low background liquid scintillation counters and high-purity germanium detectors, respectively. The atmospheric 90Sr and 137Cs concentrations decreased exponentially during 2011. The time variation of the 90Sr/137Cs ratio was obtained, and we found that the ratio rose from 1.2 × 10-3 in March to 1.3 × 10-1 in August 2011. One reason for the increase in the 90Sr/137Cs ratio could be the change in the primary emission source of activity at the FDNPP, which occurred near June 2011.

Use of a size-resolved 1-D resuspension scheme to evaluate resuspended radioactive material associated with mineral dust particles from the ground surface.

A size-resolved, one-dimensional resuspension scheme for soil particles from the ground surface is proposed to evaluate the concentration of radioactivity in the atmosphere due to the secondary emission of radioactive material. The particle size distributions of radioactive particles at a sampling point were measured and compared with the results evaluated by the scheme using four different soil textures: sand, loamy sand, sandy loam, and silty loam. For sandy loam and silty loam, the results were in good agreement with the size-resolved atmospheric radioactivity concentrations observed at a school ground in Tsushima District, Namie Town, Fukushima, which was heavily contaminated after the Fukushima Dai-ichi Nuclear Power Plant accident in March 2011. Though various assumptions were incorporated into both the scheme and evaluation conditions, this study shows that the proposed scheme can be applied to evaluate secondary emissions caused by aeolian resuspension of radioactive materials associated with mineral dust particles from the ground surface. The results underscore the importance of taking soil texture into account when evaluating the concentrations of resuspended, size-resolved atmospheric radioactivity.

Temporal changes in dissolved 137Cs concentrations in groundwater and stream water in Fukushima after the Fukushima Dai-ichi Nuclear Power Plant accident.

The concentration of dissolved 137Cs in groundwater and stream water in the headwater catchments in Yamakiya district, located ∼35 km north west of Fukushima Dai-ichi Nuclear Power Plant (FDNPP), was monitored from June 2011 to July 2013, after the earthquake and tsunami disaster. Groundwater and stream water were sampled at intervals of approximately 2 months at each site. Intensive sampling was also conducted during rainstorm events. Compared with previous data from the Chernobyl NPP accident, the concentration of dissolved 137Cs in stream water was low. In the Iboishi-yama catchment, a trend was observed for the concentration of dissolved 137Cs in stream water to decline, which could be divided into two phases by October 2011 (a fast flush of activity as a result of rapid washoff and a slow decline as a result of soil fixation and redistribution processes). The highest 137Cs concentration recorded at Iboishi-yama was 1.2 Bq/L on August 6, 2011, which then declined to 0.021-0.049 Bq/L during 2013 (in stream water under normal water-flow conditions). During the rainfall events, the concentration of dissolved 137Cs in stream water increased temporarily. The concentration of dissolved 137Cs in groundwater at a depth of 30 m at Iboishi-yama displayed a decreasing trend from 2011 to 2013, with a range from 0.039 Bq/L to 0.0025 Bq/L. The effective half-lives of stream water in the initial fast flush and secondary phases were 0.10-0.21 and 0.69-1.5 y, respectively in the three catchments. The effective half-life of groundwater was 0.46-0.58 y at Koutaishi-yama and 0.50-3.3 y at Iboishi-yama. The trend for the concentration of dissolved 137Cs to decline in groundwater and stream water was similar throughout 2012-2013, and the concentrations recorded in deeper groundwater were closer to those in stream water. The declining trend of dissolved 137Cs concentrations in stream water was similar to that of the loss of canopy 137Cs by throughfall, as shown in other reports of forest sites in the Yamakiya district.

Detection of uranium and chemical state analysis of individual radioactive microparticles emitted from the Fukushima nuclear accident using multiple synchrotron radiation X-ray analyses.

Synchrotron radiation (SR) X-ray microbeam analyses revealed the detailed chemical nature of radioactive aerosol microparticles emitted during the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, resulting in better understanding of what occurred in the plant during the early stages of the accident. Three spherical microparticles (∼2 µm, diameter) containing radioactive Cs were found in aerosol samples collected on March 14th and 15th, 2011, in Tsukuba, 172 km southwest of the FDNPP. SR-µ-X-ray fluorescence analysis detected the following 10 heavy elements in all three particles: Fe, Zn, Rb, Zr, Mo, Sn, Sb, Te, Cs, and Ba. In addition, U was found for the first time in two of the particles, further confirmed by U L-edge X-ray absorption near-edge structure (XANES) spectra, implying that U fuel and its fission products were contained in these particles along with radioactive Cs. These results strongly suggest that the FDNPP was damaged sufficiently to emit U fuel and fission products outside the containment vessel as aerosol particles. SR-µ-XANES spectra of Fe, Zn, Mo, and Sn K-edges for the individual particles revealed that they were present at high oxidation states, i.e., Fe(3+), Zn(2+), Mo(6+), and Sn(4+) in the glass matrix, confirmed by SR-µ-X-ray diffraction analysis. These radioactive materials in a glassy state may remain in the environment longer than those emitted as water-soluble radioactive Cs aerosol particles.

Initial flux of sediment-associated radiocesium to the ocean from the largest river impacted by Fukushima Daiichi Nuclear Power Plant.

This study aimed to quantify the flux of radiocesium in the Abukuma Basin (5,172 km(2)), the largest river system affected by fallout from the Fukushima Daiichi Nuclear Power Plant (FDNPP) event. In the period from 10 August 2011 to 11 May 2012 an estimated 84 to 92% of the total radiocesium transported in the basin's fluvial system was carried in particulate form. During this monitoring period Typhoon Roke (September 2011) was observed to induce a significant and temporally punctuated redistribution of radiocesium. The storm-mobilised radiocesium was an estimated 6.18 Terabecquerels corresponding to 61.4% of the total load delivered to the coastal zone during the observation period. The total flux of radiocesium into the Pacific Ocean estimated at the outlet station (basin area 5,172 km(2)) was 5.34 TBq for (137)Cs, and 4.74 TBq for (134)Cs, corresponding to 1.13% of the total estimated radiocesium fallout over the basin catchment (890 TBq). This was equivalent to the estimated amount of direct leakage from FDNPP to the ocean during June 2011 to September 2012 of 17 TBq and the Level 3 Scale Leakage on 21 August 2013 (24 TBq).

Emission of spherical cesium-bearing particles from an early stage of the Fukushima nuclear accident.

The Fukushima nuclear accident released radioactive materials into the environment over the entire Northern Hemisphere in March 2011, and the Japanese government is spending large amounts of money to clean up the contaminated residential areas and agricultural fields. However, we still do not know the exact physical and chemical properties of the radioactive materials. This study directly observed spherical Cs-bearing particles emitted during a relatively early stage (March 14-15) of the accident. In contrast to the Cs-bearing radioactive materials that are currently assumed, these particles are larger, contain Fe, Zn, and Cs, and are water insoluble. Our simulation indicates that the spherical Cs-bearing particles mainly fell onto the ground by dry deposition. The finding of the spherical Cs particles will be a key to understand the processes of the accident and to accurately evaluate the health impacts and the residence time in the environment.

Atmospheric fallout of (129)I in Japan before the Fukushima accident: regional and global contributions (1963-2005).

Atmospheric (129)I deposition was studied in different locations of Japan (Akita, Tsukuba, Tokyo, and Ishigaki Island) with samples collected between 1963 and 2005 in order to understand the distribution and sources of this nuclide and provide a reference deposition level prior to the Fukushima accident. Over this time period, the deposition pattern of (129)I in Tsukuba and Tokyo (on the Pacific side) differed from that of Akita (on the Japan Sea side). The primary source of deposition in Tsukuba and Tokyo is related to the (129)I discharge from domestic reprocessing in Tokai-mura. In contrast, the time-series pattern of deposition in Akita seems to have been influenced by (129)I discharges from reprocessing facilities in Europe and the transport of this radionuclide by westerly winds to coastlines of the Japan Sea. The (129)I deposition in Ishigaki (one of the southernmost islands in Japan) is influenced primarily by oceanic air masses (easterly winds), and deposition was 1 order of magnitude lower than that observed in Tsukuba and Tokyo. Cumulative (129)I deposition in Tokyo before the Fukushima accident was estimated at 13 mBq/m(2). The results of this study on deposition contribute to understanding the deposition levels of (129)I prior to the accident.

Variations of 129I in the atmospheric fallout of Tokyo, Japan: 1963-2003.

Atmospheric fallout samples collected from Tokyo between 1963 and 2003 were analyzed using accelerator mass spectrometry (AMS) in order to determine (129)I/(127)I ratios and to examine the deposition rate of (129)I and its secular variation in Tokyo. The (129)I/(127)I ratios in the atmosphere during 1963-1977 ranged from 1 × 10(-8) to 2 × 10(-8). This is roughly 4 orders of magnitude higher than pre-atomic levels, possibly due to atmospheric nuclear weapons tests. The calculated monthly atmospheric deposition rates of (129)I differed from those produced by nuclear fallout of (90)Sr and (137)Cs, indicating that the variations in (129)I deposition are not influenced exclusively by either nuclear bomb testing or by the Chernobyl accident. After 1978, high (129)I depositions (up to 0.13 mBq/m(2)/month) were observed. The (129)I depositions started to increase markedly at the latter half of the 1970s. The secular variation of the estimated annual (129)I deposition in Tokyo showed a close relationship between the annual atmospheric discharge of (129)I from the Tokai Reprocessing plant. Therefore, the atmospheric fallout collected from Tokyo after the late 1970s is influenced primary by the (129)I discharge from the Tokai Reprocessing plant.

Temporal variation and provenance of thorium deposition observed at Tsukuba, Japan.

Temporal variations of monthly thorium (Th) deposition observed at Tsukuba, Japan during the period 1990-2007, comparing with plutonium deposition, was studied. The monthly (232)Th deposition as did (239,240)Pu, varied according to season and inter-annually. In particular, (232)Th deposition increased significantly in spring coinciding with Asian dust (Kosa) events. The (230)Th/(232)Th activity ratios vary according to sources and can therefore be used to differentiate between locally derived and remotely derived (232)Th. The (230)Th/(232)Th activity ratios in deposition samples showed large variability with high ratios occurring in early spring. These high (230)Th/(232)Th ratios in deposition can be attributed to local dust storms, especially in early spring, that cause resuspension of soils from cultivated fields which are characterized by high (230)Th/(232)Th activity ratios. The results reveal that both locally and remotely derived (232)Th deposition showed seasonal variations with maxima in spring, although the remotely derived fraction is dominant rather than the locally derived one. The (232)Th deposition maxima later in spring is attributable to the remotely derived fraction, corresponding to the Kosa events. Annual (232)Th deposition exhibited an increasing trend, suggesting the presence of sources other than soil dust such as fly ash from increasing coal burning.

Determination of Pu isotopes and 241Am in a reference fallout material using SF-ICP-MS.

This paper reports on the characterisation of activities of Pu and (241)Am, and Pu isotopic composition in a reference fallout material prepared by the Meteorological Research Institute (MRI), Japan, from samples collected at 14 stations throughout Japan in 1963-1979. The acid leaching and total digestion were used to compare whether there is difference in Pu and (241)Am activities and Pu isotopic composition between these two methods. The results of activities of (239+240)Pu and (241)Pu, and Pu isotopic composition have been reported in the previous work (Sci. Total Environ. 2010, 408, 1139-1144). In this study, the (241)Am activity and (241)Am/(239+240)Pu activity ratio in the reference fallout material are reported, and the usefulness of Pu atom ratios and (241)Am/(239+240)Pu activity ratio for source identification is discussed.