Natural radionuclides and radiological risk assessment in the stream and river sediments of a high background natural radiation area Kanyakumari, India.

The Kanyakumari coast is known to be a high background natural radiation area due to the placer deposits of heavy minerals such as ilmenite, monazite, and rutile. The Kanyakumari river sediments that could be the source of the elevated amounts of natural radionuclides in the coastal sands have been studied in this paper. The activity concentrations of primordial radionuclides 226Ra, 232Th, and 40K were determined using high-purity germanium (HPGe) gamma-ray spectrometry. The mean activity concentrations of 226Ra, 232Th, and 40K were found to be 75 Bq kg-1, 565 Bq kg-1, and 360 Bq kg-1, respectively. The mean absorbed dose rate was 395 nGy h-1. Radiological hazard parameters were studied and compared with the world average values. The contribution of 232Th to the total dose rate was found to be higher than that of the two other radionuclides. The high mean ratio of 232Th/226Ra suggested an enrichment of 232Th and the occurrence of 226Ra leaching due to an oxidizing environment. Principal component analysis (PCA) was carried out for the radionuclides in order to discriminate the source of the sediments. This study provides new insights into the distribution of natural radionuclides in sediments of rivers and streams.

Rapid Method To Determine 137Cs, 237Np, and Pu Isotopes in Seawater by SF-ICP-MS.

Neptunium-237, owing to its long half-life (t1/2 = 2.14 × 106 year) and similar conservatism to 137Cs, has the potential to replace 137Cs for water mass circulation studies on decades and even longer time scales. A new method for the determination of 137Cs, 237Np, and Pu isotopes in seawater samples was proposed to solve the difficulty of 237Np analysis in seawater. The developed method includes the separation technique of ammonium phosphomolybdate (AMP) adsorption for 137Cs and anion exchange chromatography for 237Np and Pu, a measurement technique of gamma spectrometry for 137Cs and SF-ICP-MS for 237Np and Pu isotopes. 242Pu as a pseudo isotope dilution tracer for Np, the negligible chemical fractionation between 237Np and 242Pu of 1.02 ± 0.06 (k = 2) was obtained by implementing sophisticated control of the redox system and chromatographic elution optimization. The analytical results for the International Atomic Energy Agency Certified Reference Materials (IAEA-443) agreed with the reference values, showing chemical yields of 65-88%, U decontamination factor above 106 level, and improved sample throughput (5 days for 12 samples). Meanwhile, the lower method detection limits (MDLs) of 237Np, 239Pu, and 240Pu were 1.3 × 10-3, 0.065, and 0.15 µBq L-1 for 15 L seawater, respectively. Results obtained by the developed method can be used to evaluate the impact on the marine ecological system of the planned marine discharge of Fukushima decontaminated wastewater. Working toward that purpose, we are the first to report the 237Np activity concentration in Pacific Ocean seawater sampled near the station site, and we obtained the value of 0.122-0.154 µBq L-1.

Development of a dose estimation system for external exposure assessment at the late phase for individuals living in areas affected by the Fukushima nuclear accident.

Although the elevated ambient dose equivalent (ADE) rates in areas radiologically affected by the 2011 Fukushima nuclear plant accident decreased as time passed, the assessment of Fukushima residents' external dose is still important. A dose estimation system for external exposure assessment at the late phase for individuals living in Fukushima Prefecture was developed for this purpose. The developed system enables the estimations of external doses over the future based on an individual behavioral pattern and ADE-rate distributions from aerial monitoring data and its predicted ADE rate. To validate the system, the estimated results were compared with the measured readings of personal dosemeters. The results indicate that the developed system properly reproduced the individual external doses of subjects living in areas where the outdoor ADE rates exceeded 0.2 µSv h-1.

Distribution of strontium-90 in soils affected by Fukushima dai-ichi nuclear power station accident in the context of cesium-137 contamination.

90Sr and 137Cs activity concentrations were determined by radiometric methods in 76 soil samples (soil, litter, rain gutter deposit, and roadside sediment samples) affected by the Fukushima Dai-ichi Nuclear Power Station (FDNPS) accident and collected from the Fukushima exclusion zone. The 90Sr and 137Cs activity concentrations were in the range of 3 to 1050 Bq kg-1 (median 82 Bq·kg-1) and 0.7 to 6770 kBq·kg-1 (median 890 kBq·kg-1), respectively (decay correction date: March 15, 2011). A strong positive correlation was found between 90Sr and 137Cs activity concentration and higher mobility of 90Sr was confirmed in Japanese soil samples. The activity ratio of 90Sr/137Cs in 85% of all samples was in the range of 5.0 × 10-5 to 5.0 × 10-4 with a median of 1.2 × 10-4. From the activity ratio values it was concluded that the 90Sr released to the atmosphere was only around 0.0003-0.02 PBq which is negligible compared to the Chernobyl accident (∼10 PBq) or other nuclear accident contaminations. From the standpoints of radioecology and radiation safety, 137Cs remains the primary pollutant of the FDNPS accident.

ACTIVITY RATIO OF URANIUM IN FUKUSHIMA SOIL SAMPLES USING MULTI-COLLECTOR INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY.

The Fukushima soils have been collected from Namie and Futaba areas for the radiocaesium and uranium isotope ratio studies. The 137Cs activity concentration of soil samples ranged from 6 ± 1 to 756 ± 14 kBq/kg. The uranium isotope ratios are measured using multi collector inductively coupled plasma mass spectrometry. The activity ratio (234U/238U) of the Fukushima soils is calculated from the measured 234U/238U isotope ratio. Activity ratio varied from 0.98 to 1.02 which indicates that 234U and 238U are in secular equilibrium. The 235U/238U atomic ratio of the Fukushima soils did not show any heterogeneity compared with the natural terrestrial ratio even with high level of 137Cs in soils.

Distributions and impacts of plutonium in the environment originating from the Fukushima Daiichi Nuclear Power Plant accident: An overview of a decade of studies.

This paper reviews the current knowledge on plutonium (Pu) isotopic composition (the atom or activity ratios) and activity concentrations of 238Pu, 239Pu, 240Pu, and 241Pu resulting from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident in 2011. In this critical review, we document the characteristic values of Pu atom or activity ratios (fingerprints) and present their spatial distributions around the FDNPP site. Based on multiple Pu fingerprints (238Pu/239+240Pu activity ratio, 240Pu/239Pu atom ratio, and 241Pu/239Pu atom ratio), we clarify that Pu contamination from the FDNPP accident occurred in a restricted terrestrial area, while Pu in the Northwest Pacific Ocean is still predominately sourced from the Pacific Proving Grounds (PPG) and global fallout. Using a simple two end-member mixing model, we calculate average contributions of Pu from the FDNPP accident of 13 ± 20% (n = 180) in soil samples, 55 ± 32% (n = 38) in leaf litter samples, and 67 ± 26% (n = 129) in air dust/black substances. In the marine environment, the PPG source average contributions are 45 ± 15% (n = 76) in seawater and 42 ± 12% (n = 48) in sediments. The spatial distributions of Pu atom or activity ratios based on existing studies suggest that: 1) in the terrestrial region investigated 80 km northwest of the FDNPP site, the Pu contamination is mainly observed in an area within a 50 km distance, and 2) in the terrestrial region investigated 60 km southwest of the FDNPP site, the Pu contamination is mainly observed in an area within a 30 km distance. Studies of Cs-bearing radioactive particles indicate that Pu occurs as Pu oxide, and the fuel fragments containing Pu that were released from the reactors to the surrounding environment are associated with micron-scale Cs-bearing radioactive particles. We note that the fractionation between Pu and other radionuclides occurred after release. These new findings about the Pu fingerprints around the FDNPP site will help researchers to establish a reference background database for future environmental risk assessment and geochemical study there.

Source and distribution characteristics of 239, 240, 241Pu, 237Np and 134, 137Cs in sediments in the Northwest and Central Equatorial Pacific after the Fukushima nuclear accident.

To understand the possible influence of the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident on the deep sea, as well as the geochemical behavior and transport of radionuclides, 134Cs, 137Cs, 239, 240Pu, 241Pu, and 237Np were measured in the abyssal sediments of the Northwest Pacific (NWP) and Central Equatorial Pacific (CEP) Ocean. Data on the characteristics of these sediments obtained after the FDNPP accident are extremely rare, especially in the NWP subtropical gyre (NPSG) region. FDNPP-derived radio-Cs (134Cs, 137Cs) arrived at the open sea floor of the NWP before 2018 but was only found in the Kuroshio-Oyashio Extension (KOE) region. No FDNPP-derived Pu was detected in the abyssal sediments of the NWP or CEP. Pu in the NWP mainly originated from global fallout and the Pacific Proving Ground (PPG) close-in fallout, except for at station WP1 (39°N in the KOE region), where an abnormal but non-FDNPP-derived Pu signal was detected. Pu in the eastern CEP sediment was less affected by the PPG close-in fallout from the Marshall Islands and was mainly derived from global fallout, with some close-in fallout from the Johnston Atoll test. The KOE region was the area most affected by PPG close-in fallout Pu via Kuroshio transport, while the lowest inventories of 239+240Pu and 237Np were found in the NPSG region due to its oligotrophic environment. The 237Np originated from the same source as Pu, and the latitudinal pattern of 237Np was consistent with that of Pu. Station SS (in the marginal sea of the NWP) contained high 237Np/239Pu atom ratios in the deeper layers of sediment and had a 237Np depth profile opposite that of the 239+240Pu profile, compared to other stations; these differences are mainly attributed to differences in the behaviors of 237Np and 239Pu.

Factors controlling dissolved 137Cs activities in coastal waters on the eastern and western sides of Honshu, Japan.

The distributions of dissolved 137Cs in river, nearshore, and offshore waters on the east and west coasts of the Japanese island of Honshu were studied in 2018-2021, 7-10 years after the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. On the east side along the north western North Pacific (Fukushima Prefecture), estuarine processes, including desorption from riverine particles and dissolution into pore water from riverine particles that had settled to the seafloor, contributed to the maintenance of high dissolved 137Cs activities in nearshore and offshore waters. A survey and mass-balance calculation in a semi-enclosed estuarine area, the Matsukawa-ura, in the northern part of Fukushima, provided convincing evidence that rivers contributed to the influx of 137Cs to coastal waters. In contrast, the extremely low activities of dissolved and particulate 137Cs in the Tedori River of Ishikawa Prefecture on the western side of Japan along the Japan Sea suggested that inputs of riverine 137Cs made a negligible contribution to the increase of dissolved 137Cs activities in the nearshore and offshore waters. The relatively high dissolved 137Cs activities observed in the offshore waters of the Japan Sea were due to movement of FDNPP-derived 137Cs into the Japan Sea via the Tsushima Warm Current. Mechanisms controlling the distributions of 137Cs activities in coastal waters of the eastern and western sides of Japan therefore differ.

Rapid analysis of 237Np and Pu isotopes in small volume urine by SF-ICP-MS and ICP-MS/MS.

Internal contamination with alpha-particle emitting actinides, such as 237Np, 239Pu, 240Pu, is likely to bring a large amount of dose to the tissues of persons even if the intake amount is small. To provide timely information for prompt decision-making in radiation emergency therapy, we developed a simple and rapid method for urinary bioassay to determine ultra-trace 237Np and Pu isotopes using SF-ICP-MS and ICP-MS/MS. To avoid polyatomic interferences and tailing effects from U, 237Np and Pu isotopes were collected after removing U effectively using a simple single chromatographic column packed with 2 mL AG MP-1M anion exchange resin, exhibiting a high decontamination factor of 108 for 238U. The overall chemical fractionation between 237Np and 242Pu for the whole analytical procedure was 0.974 ± 0.064 (k = 2), allowing us to measure 237Np and Pu isotopes using 242Pu as a yield tracer with yields of 76 ± 5%. Using ICP-MS/MS with low background provided the method detection limits for 237Np, 239Pu, 240Pu, and 241Pu of 0.025, 0.025, 0.015, and 0.020 fg mL-1, respectively, for 20 mL of urine sample. Those were comparable to detection limits of SF-ICP-MS with high sensitivity. Subsequently, three urine reference materials with Pu spike, provided by the Association for the PROmotion of Quality COntrol in RADiotoxicological Analysis (PROCORAD), France, were analyzed by the developed method and the conventional alpha spectrometry technique for validation. Finally, the developed method was successfully employed to measure the contamination level of 237Np, 239Pu, 240Pu, and 241Pu in urine samples collected during decorporation therapy using DTPA, after a Pu inhalation exposure accident in Japan. The high throughput (9 h for 12 samples), simplicity, low cost, and high sensitivity of the method will allow greater numbers of related laboratories to be involved in screening activities for unexpected actinide exposure, such as in the case of a large scale radiological disaster.

A Microwave Digestion Technique for the Analysis of Rare Earth Elements, Thorium and Uranium in Geochemical Certified Reference Materials and Soils by Inductively Coupled Plasma Mass Spectrometry.

Two different digestion methods-microwave digestion (Mw) and Savillex digestion (Sx)-were used to evaluate the best quality control for analysis of the rare earth elements, Th and U in the geochemical certified reference material JSd-2, supplied by the Geological Survey of Japan (GSJ). The analysis of trace elements was carried out using inductively coupled plasma mass spectrometry (ICP-MS). The digestion recovery was > 90% for almost all elements by both methods. Mw-4 (four repeats of the microwave digestion) was found to be more effective and faster than Sx. In order to evaluate the efficiency of Mw-4, three other GSJ certified reference materials, JLk-1, JB-1 and JB-3, as well as five different soil samples from Belarus, Japan, Serbia and Ukraine were also analyzed. The Mw-4 method was seen to be promising for complete digestion and recovery of most of the elements. The U/Th ratio showed some heterogeneity for Ukraine and Serbia soils affected by Chernobyl nuclear power plant accident and depleted uranium contamination, respectively. This method can be successfully applied to any type of soils for elemental analyses.

Behavior of Radiocesium in Sediments in Fukushima Coastal Waters: Verification of Desorption Potential through Pore Water.

Concentrations of 137Cs in seawater, seabed sediment, and pore water collected from the area around Fukushima were investigated from 2015 to 2018, and the potential of coastal sediments to supply radiocesium to the bottom environment was evaluated. The 137Cs concentration in the pore water ranged from 33 to 1934 mBq L-1 and was 10-40 times higher than that in the overlying water (seawater overlying within 30 cm on the seabed). At most stations, the 137Cs concentrations in the overlying water and the pore water were approximately proportional to those in the sediment. The conditional partition coefficient between pore water and sediment was [0.9-14] × 102 L kg-1, independent of the year of sampling. These results indicated that an equilibrium of 137Cs between pore water and sediment has been established in a relatively short period, and 137Cs in the pore water is gradually exported to seawater near the seabed. A simple box model estimation based on these results showed that 137Cs in the sediment decreased by about 6% per year by desorption/diffusion of 137Cs from the seabed.

Changing Emotions About Fukushima Related to the Fukushima Nuclear Power Station Accident-How Rumors Determined People's Attitudes: Social Media Sentiment Analysis.

BACKGROUND: Public interest in radiation rose after the Tokyo Electric Power Company (TEPCO) Fukushima Daiichi Nuclear Power Station accident was caused by an earthquake off the Pacific coast of Tohoku on March 11, 2011. Various reports on the accident and radiation were spread by the mass media, and people displayed their emotional reactions, which were thought to be related to information about the Fukushima accident, on Twitter, Facebook, and other social networking sites. Fears about radiation were spread as well, leading to harmful rumors about Fukushima and the refusal to test children for radiation. It is believed that identifying the process by which people emotionally responded to this information, and hence became gripped by an increased aversion to Fukushima, might be useful in risk communication when similar disasters and accidents occur in the future. There are few studies surveying how people feel about radiation in Fukushima and other regions in an unbiased form. OBJECTIVE: The purpose of this study is to identify how the feelings of local residents toward radiation changed according to Twitter. METHODS: We used approximately 19 million tweets in Japanese containing the words "radiation" (), "radioactivity" (), and "radioactive substances" () that were posted to Twitter over a 1-year period following the Fukushima nuclear accident. We used regional identifiers contained in tweets (ie, nouns, proper nouns, place names, postal codes, and telephone numbers) to categorize them according to their prefecture, and then analyzed the feelings toward those prefectures from the semantic orientation of the words contained in individual tweets (ie, positive impressions or negative impressions). RESULTS: Tweets about radiation increased soon after the earthquake and then decreased, and feelings about radiation trended positively. We determined that, on average, tweets associating Fukushima Prefecture with radiation show more positive feelings than those about other prefectures, but have trended negatively over time. We also found that as other tweets have trended positively, only bots and retweets about Fukushima Prefecture have trended negatively. CONCLUSIONS: The number of tweets about radiation has decreased overall, and feelings about radiation have trended positively. However, the fact that tweets about Fukushima Prefecture trended negatively, despite decreasing in percentage, suggests that negative feelings toward Fukushima Prefecture have become more extreme. We found that while the bots and retweets that were not about Fukushima Prefecture gradually trended toward positive feelings, the bots and retweets about Fukushima Prefecture trended toward negative feelings.

Suspended Particle-Water Interactions Increase Dissolved 137Cs Activities in the Nearshore Seawater during Typhoon Hagibis.

Distributions of 137Cs in dissolved and particulate phases of the downstream reaches of seven rivers and adjacent nearshore and offshore waters as far as ∼60 km south of the Fukushima Dai-ichi nuclear power plant (FDNPP) were studied during the high-river-flow period (June-September 2019) and during the period of October 2019 after typhoon Hagibis. Dissolved 137Cs activities in nearshore water were higher than those in rivers and offshore waters, and this distribution was more intensified after the typhoon, indicating the desorption of 137Cs from riverine suspended particles in addition to the ongoing release of contaminated water from the FDNPP and re-entry of radiocesium via submarine groundwater discharge. This scenario is also supported by the reduction of distribution coefficient (Kd) from a geometric mean value of 5.5 × 105 L/kg in rivers to 9.8 × 104 L/kg in nearshore water. The occupation of desorbed 137Cs to the dissolved activity of this nuclide in nearshore water was estimated to be 0.7%-20% (median: 9.7%) during the high-river-flow period, increasing to 1.4%-66% (32.3%) after the typhoon, suggesting that the desorption during the flood period such as typhoons further contributes to the increase in dissolved 137Cs levels in nearshore water.

Chemical Separation of Uranium and Precise Measurement of 234U/238U and 235U/238U Ratios in Soil Samples Using Multi Collector Inductively Coupled Plasma Mass Spectrometry.

A new chemical separation has been developed to isolate uranium (U) using two UTEVA columns to minimize iron and thorium interferences from high background area soil samples containing minerals like monazites and ilmenite. The separation method was successfully verified in some certified reference materials (CRMs), for example, JSd-2, JLk-1, JB-1 and JB-3. The same method was applied for purification of U in Fukushima soil samples affected by the Fukushima dai-ichi nuclear power station (FDNPS) accident. Precise and accurate measurement of 234U/238U and 235U/238U isotope ratios in chemically separated U were carried out using a multi-collector inductively coupled plasma mass spectrometer (MC-ICP-MS). In this mass spectrometric method, an array of two Faraday cups (1011 Ω, 1012 Ω resistor) and a Daly detector were simultaneously employed. The precision of U isotope ratios in an in-house standard was evaluated by replicate measurement. Relative standard deviation (RSD) of 234U/238U and 235U/238U were found to be 0.094% (2σ) and 0.590% (2σ), respectively. This method has been validated using a standard reference material SRM 4350B, sediment sample. The replicate measurements of 234U/238U in SRM shows 0.7% (RSD). This developed method is suitable for separation of U and its isotope ratio measurement in environmental samples.

Precise Measurement of Tellurium Isotope Ratios in Terrestrial Standards Using a Multiple Collector Inductively Coupled Plasma Mass Spectrometry.

Precise tellurium (Te) isotope ratio measurement using mass spectrometry is a challenging task for many decades. In this paper, Te isotope ratio measurements using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) in terrestrial Te standards have been reported. Newly developed Faraday cup with 1012 Ω resistor is used to measure low abundance 120Te, whereas the 1011 Ω resistor is used to measure other Te isotopes. The relative standard deviation obtained for Te isotope ratio measurement by Faraday cups of 120Te/128Te [0.002907(05)], 122Te/128Te [0.079646(10)], 123Te/128Te [0.027850(07)], 125Te/128Te [0.221988(09)], 126Te/128Te [0.592202(20)], and 130Te/128Te [1.076277(30)] were 0.140%, 0.014%, 0.026%, 0.005%, 0.004%, and 0.004%, respectively. The measured isotope ratio results are compared with previous results obtained by thermal ionization mass spectrometry (TIMS), negative thermal ionization mass spectrometry (N-TIMS), and MC-ICP-MS, showing an improvement in the precision about one order of magnitude for 120Te/128Te ratio. The present study shows better precision for Te isotope ratios compared to earlier studies.

129I in a sediment core offshore Fukushima: Distribution, source and its implication.

129I released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has been observed in the atmospheric, terrestrial and oceanic environments, and it also entered the marine sediments via dispersion by sea water movement and deposition around Japan. However, there have been few studies of marine sediment cores in contrast to the large number of studies on seawater. In this work, a sediment core collected near FDNPP was analyzed for 129I. It is observed that the 129I/127I atomic ratios in this sediment core are comparable to those in the seawater and sediments collected from offshore Fukushima after the accident, but 2 orders of magnitude higher than those in seawater in this region before the accident, suggesting the significant amount of 129I has been transferred and incorporated to the offshore shallow sediments. The difference in environmental behavior between 129I and 137Cs is discussed based on their depth distributions in the sediment core in comparison with the grain size distribution of sediments. The peak concentrations of iodine isotopes were found in a relatively deeper layer than radiocesium. Radiocesium follows the distribution of fine grains in the sediment core, implying its high association to fine grains.

Reconstruction of radiocesium levels in sediment off Fukushima: Simulation analysis of bioavailability using parameters derived from observed 137Cs concentrations.

Radiocesium was released to the North Pacific coastal waters by the accident at the Fukushima Dai-ichi Nuclear Power Plant (1FNPP) of the Tokyo Electric Power Company (TEPCO) in March 2011. Since the radiocesium in the sediment off Fukushima was suggested as a possible source for the transfer of this radionuclide through the benthic food chain, we conducted numerical simulations of 137Cs in sediments off the Fukushima coast by using a model which incorporates dynamic transfer processes between seawater and the labile and refractory fractions in sediment particles. This model reproduced the measured temporal changes of 137Cs concentration in seabed surface sediment off Fukusima coasts, by normalizing the radiocsium transfer between seawater and sediment according to the particle diameter sizes. We found that the 137Cs level in sediment decreased by desorption during the first several months after the accident, followed by a reduction in the labile fraction until the end of 2012. The apparent decrease of the total radiocesium level in surface sediment was estimated to occur at rates of approximately 0.2 y-1 within a 20 km distance from the 1FNPP. The comparison of 137Cs level decreases in the demersal fish and the simulated temporal labile fraction in fine sediment demonstrated that the consideration of radiocesium transfer via sediment is important for determining the 137Cs depuration mechanism in some demersal fish.

Accurate and precise determination of 90Sr at femtogram level in IAEA proficiency test using Thermal Ionization Mass Spectrometry.

A novel method for the determination of ultra-trace level 90Sr has been recently developed applying thermal ionization mass spectrometry (TIMS). The method includes the chemical separation of Zr (isobaric interference of 90Zr) from the samples followed by determination of 90Sr/88Sr abundance  sensitivity (2.1 × 10-10). The analytical performance of this method was assessed in the IAEA-TEL 2017-3 worldwide open proficiency test. For 90Sr determination, tap water and milk powder samples were distributed amongst the participant laboratories with reference values of 11.2 ± 0.3 Bq kg-1 (2.2 ± 0.1 fg g-1) and 99.9 ± 5.0 Bq kg-1 (19.5 ± 1.0 fg g-1), respectively. The stable Sr concentrations were 39.4 ± 0.9 ng g-1 and 2.5 ± 0.1 µg g-1 while the 90Sr/88Sr isotope ratios were 6.47 ± 0.17 × 10-8 and 9.04 ± 0.45 × 10-9 in the tap water and milk powder samples, respectively. For TIMS measurement, 50 mL water and 1 g milk powder samples were taken for analysis. This TIMS method demonstrated an impressive accuracy (relative bias of 4.2% and -2.1%, respectively) and precision (relative combined uncertainty of 4.1% and 7.6%, respectively) when compared with radiometric techniques. For the first time in the history of inorganic mass-spectrometry, 90Sr analysis using a TIMS instrument is confirmed by an independent proficiency test.

First determination of Pu isotopes (239Pu, 240Pu and 241Pu) in radioactive particles derived from Fukushima Daiichi Nuclear Power Plant accident.

Radioactive particles were released into the environment during the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. Many studies have been conducted to elucidate the chemical composition of released radioactive particles in order to understand their formation process. However, whether radioactive particles contain nuclear fuel radionuclides remains to be investigated. Here, we report the first determination of Pu isotopes in radioactive particles. To determine the Pu isotopes (239Pu, 240Pu and 241Pu) in radioactive particles derived from the FDNPP accident which were free from the influence of global fallout, radiochemical analysis and inductively coupled plasma-mass spectrometry measurements were conducted. Radioactive particles derived from unit 1 and unit 2 or 3 were analyzed. For the radioactive particles derived from unit 1, activities of 239+240Pu and 241Pu were (1.70-7.06) × 10-5 Bq and (4.10-8.10) × 10-3 Bq, respectively and atom ratios of 240Pu/239Pu and 241Pu/239Pu were 0.330-0.415 and 0.162-0.178, respectively. These ratios were consistent with the simulation results from ORIGEN code and measurements from various environmental samples. In contrast, Pu was not detected in the radioactive particles derived from unit 2 or 3. The difference in Pu contents is clear evidence towards different formation processes of radioactive particles, and detailed formation processes can be investigated from Pu analysis.

Dose rate estimation of freshwater wildlife inhabiting irrigation ponds in the exclusion zone of the Fukushima Dai-ichi Nuclear Power Plant accident.

To assess the risks of ionising radiation to freshwater environments in the exclusion zone of the Fukushima Dai-ichi Nuclear Power Plant accident, the absorbed dose rates to aquatic organisms possibly inhabiting the irrigation ponds were estimated using the ERICA Assessment Tool from 134Cs and 137Cs radioactivity monitoring data for the period 2013 to 2017. In each year, the total dose rates to benthic organisms were in the same or higher levels compared with those to pelagic organisms. Among pelagic organisms, the total dose rates to amphibians, birds, and pelagic fish were two orders of magnitude higher than those to plankton. The total dose rates to insect larvae, which attained a maximum of 130 µGy h-1, were higher than those to the other benthic organisms. The dose rates to benthic organisms increased from 2013 to 2015 and remained constant thereafter. In 50-93% of ponds, the dose rates to at least one taxon of freshwater organism, all of which were benthic organisms, exceeded the ERICA screening level (10 µGy h-1). Comparison of the estimated dose rates with the ICRP's derived consideration reference levels (DCRLs) suggests that radioactive contamination was not likely to damage amphibians, birds, pelagic fish, benthic fish, crustaceans, and insect larvae inhabiting most of the irrigation ponds in the exclusion zone. However, this comparison also suggests that there was some chance of deleterious effects occurring to birds and benthic fish in a limited number of the most severely contaminated irrigation ponds.