Measurement of fallout with rain in Hiroshima and several sites in Japan from the Fukushima reactor accident

Fallout with rain from the Fukushima reactor accident was monitored for about two months in Higashi-Hiroshima City, Hiroshima, Japan, from March 20 to May 23, 2011. Gamma-ray (γ-ray) spectra measured using a low background HPGe spectrometer showed clear evidence of fission products—¹³¹I, ¹³⁷Cs, and ¹³⁴Cs. The ¹³¹I was observed on March 27 and April 8, while ¹³⁷Cs and ¹³⁴Cs were observed on March 27, April 18, and April 22. The ¹³¹I, ¹³⁷Cs, and ¹³⁴Cs activity concentrations in rainwater collected in Hiroshima reached 0.44 ± 0.09 on April 8, 0.17 ± 0.01 on April 18, and 0.15 ± 0.01 Bq/L on April 18, 2011, respectively. These activity levels were compared with global results collected from the Northern Hemisphere. Several samples of rainwater that were collected in Chiba (Kashiwa) on March 21, April 11, and May 12; Tokyo (Nerima) on March 21 and April 11; Osaka (Hirano) on April 8; Nara (Kitakatsuragi) on April 9; and Fukushima (Fukushima) on April 19, were also measured by our spectrometer and compared. Among these samples of rainwater collected at different locations in Japan, the one collected at Kashiwa City, Chiba Prefecture, on March 21 showed the highest activity concentrations of 6072 ± 1,   632 ± 4,   766 ± 3,   637 ± 1,   97.6 ± 0.8, and 752 ± 2 Bq/L for ¹³¹I,   ¹³²I,   ¹³²Te,   ¹³⁴Cs,   ¹³⁶Cs, and ¹³⁷Cs, respectively. The health risks due to these high activity levels were considered in terms of several regulations. The ratio of the activites for the isotopes ¹³¹I to ¹³⁷Cs and ¹³⁴Cs to ¹³⁷Cs were compared with the other measurements and discussed.     

Radionuclides from Fukushima accident in Thessaloniki, Greece (40°N) and Milano, Italy (45°)

¹³¹I, ¹³⁷Cs and ¹³⁴Cs were observed in environmental samples in Milano (40°N), Italy and Thessaloniki (45°N), Greece, soon after the nuclear accident in Fukushima, Japan. The radionuclide concentrations were determined and studied as a function of time. In Thessaloniki the ¹³¹I in air was observed for the first time on March 24, 2011. In Milano, the first evidence of Fukushima fallout has been confirmed with ¹³¹I and ¹³⁷Cs measured in wet precipitation collected 2 days later. The maximum ¹³¹I activity concentration in air of 467 ± 25 μBq m^?3, observed in Milano on April 3–4, 2011, was almost similar to the highest value of 497 ± 53 μBq m^?3 observed in Thessaloniki. The ¹³⁴Cs/¹³⁷Cs activity ratio values in air were around 1 in both regions. Soil, grass and milk samples were contaminated with ¹³¹I and ¹³⁷Cs at a low level. Finally, a dose assessment for these two areas showed clearly that the detected activities in all environmental samples were far below levels of concern.     

Environmental radioactivity measurements in north–western Greece following the Fukushima nuclear accident

The impact of the Fukushima nuclear accident in north–western Greece was assessed through an environmental monitoring programme activated by the Nuclear Physics Laboratory of the University of Ioannina. Measurements of ¹³¹I were carried out in atmospheric particulate, ovine milk and grass samples. In daily aerosol samplings, radioiodine was first detected on March 25–26, 2011 and reached maximum levels, up to 294 μBq m^?3, between April 2 and April 4, 2011. In ovine milk samples, ¹³¹I concentrations ranged from 2.0 to 2.7 Bq L^?1 between April 2 and April 6, 2011, while an average activity of 2.7 Bq kg^?1 was measured in grass samples on April 4, 2011. The ^134,137Cs isotopes were below detection limits in all samples and could only be determined in the air, by analysis of multiple daily filters. A maximum average activity concentration of ¹³⁷Cs amounting to 24 μBq m^?3 was measured during the period from April 5 to April 9, 2011, with the ¹³⁴Cs/¹³⁷Cs activity ratio being close to unity. Activity concentrations were consistent with measurements conducted in other parts of the country and were well below those reported in May 1986 after the Chernobyl accident. The committed effective dose to the whole body and to the thyroid gland from inhalation of ¹³¹I was estimated for the adult and infant population and was found to be of no concern for the public health.     

Determination of131I,134Cs,137Cs in grass and cheese after Chernobyl accident in Austria

Various samples from Styria /grass/ and Salzburg /cheese/ were analyzed for¹³¹I,¹³⁴Cs and¹³⁷Cs concentration during April–July 1986 by -ray spectrometry. The concentrations are reported in nCi kg^–1 wet weight. The concentration values found for¹³¹I 0.2–17.2 nCi kg^–1 /grass/, 0.1–0.5 nCi kg^–1 /cheese/, for¹³⁴Cs 1.1–6.2 nCi kg^–1 /grass/, 0.2–1.3 nCi kg^–1 /cheese/, for¹³⁷Cs 1.6–15.7 nCi kg^–1 /grass/, 0.3–2.2 nCi kg^–1 /cheese/. While radioactivity of¹³¹I,¹³⁴Cs and¹³⁷Cs in cheese samples increases from May to June, it decreases in grass samples from May to July 1986.     

Determination of131I,134Cs,137Cs in plants and cheese after Chernobyl accident in Roumania

Various samples from the south-east region of Roumania/greens, fodder, cheese/were analyzed for¹³¹I,¹³⁴Cs and¹³⁷Cs concentrations in May and July 1986 by -ray spectrometry. The concentrations are reported in nCi. kg^–1 wet weight. For greens, a considerable decrease was observed for¹³¹I/to 3.0–7.0 nCi. kg^–1/,¹³⁴Cs/to 0.5–2.0 nCi.kg^–1/ and¹³⁷Cs /to 1.0–4.0 nCi. kg^–1/ from the first half /5–15 May/ till the end of May 1986. For cheese, maximum values were measured between 5 and 15 May /sheep cottage cheese: 500–800 nCi.kg^–1 for¹³¹I, 25–50 nCi. kg^–1 for¹³⁴Cs, 40–80 nCi. kg^–1 for¹³⁷Cs/; at the beginning of July a considerable decrease /to 5–10 nCi. kg^–1 for¹³¹I, 1.2–2.0 nCi.kg^–1 for¹³⁴Cs, 2.2–3.0 nCi. kg^–1 for¹³⁷Cs/ was observed. In autumn 1986 a small increase up to 2.0–3.0 nCi. kg^–1 for¹³⁴Cs and 3.4–5.0 nCi. kg^–1 for¹³⁷Cs /in November/ was reported. The population's internal possible contamination was strongly limited by the authorities' severe control of the food-stuff.     

The study on radioactive contamination in foodstuffs imported from Japan after the Fukushima accident

During the Fukushima nuclear accident, a large number of radionuclides were released, causing direct radioactive contamination to the environment and the ecosystem, and eventually indirect contamination to the foodstuffs. The Radiation Monitoring Group, Office of Atoms for Peace (OAP) in cooperation with the Food and Drug Administration (FDA), has been monitoring the foodstuffs imported from Japan, especially the Fukushima and nearby areas. This monitoring program covered the potentially contaminated foodstuffs. The measurements were mainly conducted using Gamma spectroscopy systems in order to analyze the radioactive concentration of ¹³¹I, ¹³⁴Cs, and ¹³⁷Cs fission products. From 442 samples collected between after the nuclear accident to the end of September 2012, 28 of contaminated food products of fission isotopes have been found with the contamination ranges of 0.63–15.25 Bq/kg fresh, 1.45–44.70 Bq/kg fresh, and 0.45–51.10 Bq/kg fresh) for ¹³¹I, ¹³⁴Cs, and ¹³⁷Cs, respectively. However, the contamination levels are still well under the Thailand standard of food contaminated with radionuclide and the relevant international standards. Finally, the research also investigated the relationship between the times the samples were collected and the contamination levels.     

Measurement of 137Cs in the soil in Korea by low-level background gamma-ray spectrometer

¹³⁷Cs was measured in soil samples collected in Korea from 2006 to 2008 using a low-level background gamma-ray spectrometer that was designed and developed by KRISS (Korea Research Institute of Standards and Science). The objectives of this study are to evaluate the newly developed low-level background gamma-ray spectrometer and, consequently, to provide information on the horizontal and vertical distribution of ¹³⁷Cs in Korean soil. ¹³⁷Cs concentrations in surface soil varied from 12.8 ± 0.9 to 108 ± 4 Bq kg^?1, and the vertical profiles of ¹³⁷Cs from the Nari basin in Ulleung Island in the East Sea/Sea of Japan and Seongsan Ilchulbong Peak, Jeju Island, showed a higher concentration in the surface layer that gradually decreased with depth. On the other hand, the ¹³⁷Cs concentration in soil samples collected from Bukhan Mountain National Park in Seoul showed a subsurface maximum and decreased with depth. The ¹³⁷Cs inventories in the soil column were calculated to be 1,830–4,360 Bq m^?2 with a mean of 2,770 Bq m^?2, which was the same order of magnitude as the global fallout inventories in the mid-latitude region of the Northern Hemisphere.     

131I,134Cs and137Cs concentrations in 1986 for some Roumanian foodstuffs

Results of post-Chernobyl measurement on some foodstuff samples /eggs, meat, fruit, honey, medicinal herbs/ from South-Eastern Roumania are presented. Gamma-ray spectrometry was used; the radioactive concentration values are given in nCi.kg^–1 wet weight. A strong decrease in concentrations for eggs from 6–7 May /3.0–7.4 nCi for¹³¹I, 0.25–0.40 nCi for¹³⁴Cs, 0.40–0.85 nCi for¹³⁷Cs per one egg, mainly in the yolk/ to 19–25 May /0.3–1.0 nCi for¹³¹I, 0.15–0.25 nCi for¹³⁴Cs, 0.25–0.40 nCi for¹³⁷Cs/ was observed. The mean values for lamb meat /joint muscle/ were 500 nCi.kg^–1 for¹³¹I, 12 nCi.kg^–1 for¹³⁴Cs, 22 nCi.kg^–1 for¹³⁷Cs /18–25 May/. Relatively reduced values were found for fruits, e.g. compared to dairy products¹. In May–June 1986, the food consumption in Roumania was strictly limited and controlled by competent authorities.     

Fukushima-derived radionuclides in ground-level air of Central Europe: a comparison with simulated forward and backward trajectories

Results of forward and backward modeling of air mass transport from Fukushima Daiichi nuclear power plant to Slovakia were compared with aerosol radioactivity measurements. Several radionuclide maxima (¹³¹I, ¹³⁴Cs and ¹³⁷Cs) were observed in the Bratislava ground-level air in March–April 2011. The ¹³¹I/¹³⁷Cs activity ratio records showed the presence of two different fresh air masses in the Bratislava air, supported by simulations of forward and backward trajectories between Fukushima and Bratislava.     

Airborne gamma-ray emitters from Fukushima detected in New York State

An air-sampling network that operates continuously as part of New York State’s environmental surveillance program collected radionuclides emitted as a result of the Fukushima nuclear accident. Samples were collected, typically for 7 days each, by drawing ~600 m³ of air through a particulate-collecting filter followed in series by a canister containing activated charcoal. Additional air sampling was implemented at ~3-day intervals at two locations. Gamma-ray spectroscopy was used to confirm the detection of ¹³¹I, ¹³⁷Cs, ¹³⁴Cs, and ⁷Be in the particulate phase at all sites, with maximum concentrations near 1,260, 160, 160, and 5,200 μBq/m³, respectively. Gas-phase ¹³¹I, collected on activated charcoal, exhibited a maximum concentration of 3,400 μBq/m³ at the sites. Assessment of radionuclide levels in the air samples suggests that there were minimal health impacts from the airborne radionuclides as the activities contributed an insignificant amount to the annual human dose.     

Semi-quantitative analysis of leaf surface contamination by radioactivity from the Fukushima Daiichi nuclear power plant accident using HPGe and imaging plate

After the nuclear power plant accident at Fukushima Daiichi on 11 March 2011, green-leaves from trees, dead-leaves and grass on ground were collected from March to June 2011 in Japan. Radioactive concentrations were measured by a high purity germanium detector. Five radionuclides including ^129mTe, ¹³²Te, ¹³¹I, ¹³⁴Cs and ¹³⁷Cs were detected. The fission product concentration of the dead-leaves was higher than those of the green-leaves in many cases. The highest concentration observed was found on the dead-leaves collected at Iwaki, 60 km far from Fukushima Daiichi. A total activity of 2,000 Bq g^?1 was measured for all 5 radionuclides. Clear images of radioactivity of the highly contaminated leaves were obtained with an imaging plate (IP) after <24 h exposure time without using a shielded box. The photostimulated luminescence values (PSL) of leaves arranged on half size of IP were roughly in proportion to their activities except for the low activity samples. Semi-quantitative analysis was possible by using PSL values with a large region of interest of half size of IP, because the radioactivity released in the case of the nuclear power plant accident was uniform in the early days.     

Extraction of cesium in seawater off Japan using AMP-PAN resin and quantification via gamma spectroscopy and inductively coupled mass spectrometry

The March 2011 earthquake off the Japanese coast and subsequent tsunami that devastated the Fukushima Dai-Ichi nuclear power plant resulted in the largest accidental release of cesium 137 and 134 to the oceans. Seawater samples were collected in June 2011 from 30 to 600 km off the coast of Japan as part of initial mapping of the spread of contamination in the ocean. Cesium was extracted from unfiltered and filtered (<1.0 μm) seawater using an absorber based upon an organic polymer polyacrylonitrile (PAN) containing ammonium molybdophosphate (AMP) Sebesta and Stefula (J Radioanal Nucl Chem 140:15–21, 1990). The AMP-PAN resin can be counted directly using gamma spectroscopy for ¹³⁴Cs and ¹³⁷Cs. Stable ¹³³Cs was added to evaluate extraction efficiency and quantified by ICP-MS. Our 5 mL AMP-PAN resin column was on average 95 % efficient in the removal of cesium from 20 L samples at an average flow rate of 35 mL min^?1. Measured activities of ¹³⁴Cs and ¹³⁷Cs ranged from a few Bq m^?3 to >300 Bq m^?3. The extraction column can be adapted to different sample volumes and easily used in the field.     

238Pu, 239+240Pu, 241Am, 90Sr and 137Cs in mountain soil samples from the Tatra National Park (Poland)

Activity concentrations and inventory for ²³⁸Pu, ^239+240Pu, ²⁴¹Am, ⁹⁰Sr, and ¹³⁷Cs in soil from Tatra Mountains of Poland are presented. Soil samples were collected using 10 cm diameter cores down to 10 cm and sliced into 3 slices. Details of the applied procedure are described with the quality assurance program. The maximum activity concentrations found for various samples were: 1782±13 Bq/kg, 17.4±0.9 Bq/kg, 3.4±0.3 Bq/kg and 84±7 Bq/kg for ¹³⁷Cs, ^239+240Pu, ²⁴¹Am and ⁹⁰Sr, respectively. The maximum cumulated deposition of ^239+240Pu is 201±8 Bq/m². The origin of radionuclides is discussed, based mostly on the observed isotopic ratio of Pu. Significant correlations were found between ^239+240Pu, ²⁴¹Am and ¹³⁷Cs. The effective vertical migration rate seems to be in the order of: ⁹⁰Sr≫Pu>Am>Cs.     

Radionuclides in redistributed sediments and ash from the Las Conchas fire in Northern New Mexico

The 2011 Las Conchas fire burned 632 km² of ponderosa pine forests and piñon–juniper woodlands in the Jemez Mountains in north central New Mexico. In the weeks following the fire, heavy rainfall caused extensive flooding and erosion of surface soil and ash from the affected areas. Samples from mud and ash flows were collected and analyzed for ¹³⁷Cs and Pu, which were originally deposited as global fallout during the era of atmospheric nuclear testing. The mean concentrations for ²³⁸Pu, ^239,240Pu and ¹³⁷Cs were 0.18 ± 0.05, 4.16 ± 1.95, and 111 ± 56 mBq/g, respectively. ^239,240Pu and ¹³⁷Cs are significantly elevated above non-fire affected regional background levels.     

Geochemical studies on the Chernobyl radioactivity in environmental samples

Artificial radionuclides in deposition and airborne dust samples in 1986 were measured at Tsukuba and 11 stations in Japan. In May 1986, the Chernobyl radioactivity was observed in rain and air samples in Japan. The Chernobyl-derived Pu isotopes, which are characterized by higher²³⁸Pu/^239,240Pu (85) and²⁴¹Pu/²³⁸Pu (0.5) activity ratios than those of the nuclear test-derived Pu and⁹⁰Sr, were detected in deposition and airborne dust samples in Japan, as well as volatile radionuclides such as¹³¹I and¹³⁷Cs. However, the activities of Pu isotopes and⁹⁰Sr observed in Japan were about two and three orders of magnitude lower than those expected from the activity ratios in the total release at Chernobyl, which means that the residence time of Pu in the air was shorter than that of¹³⁷Cs. In order to understand the fractionation between the Chernobyl radionuclides we studied about individual wet and dry deposition. The results suggest that this cause is due to the difference of the particle size of radionuclide-bearing particles, which may be related to the release process of Chernobyl radionuclides.     

Plutonium isotopes and 137Cs in Dolon settlement near the Semipalatinsk Nuclear Test Site: About 50 years after the first nuclear weapon testing

Recent controversies concerning the radiation doses for populations living in the village of Dolon due to the nuclear explosions carried out at the Semipalatinsk Nuclear Test Site (SNTS) have encouraged us to evaluate in more detail the levels and distributions of residual long-lived radionuclides¹³⁷Cs and Pu isotopes (²³⁸Pu,^239,240Pu) in soils within the village. Soil core samples up to a depth of about 30 cm and/or 100 cm were collected at 25 sites and subjected to analysis of ¹³⁷Cs and Pu isotopes. The inventories of ¹³⁷Cs and ^239,240Pu were found to be in the wide range of 790-10,310 and 530-14,320 Bq/m², respectively. Sequential leaching of Pu from the soil showed that more than ca. 80% of the ^239,240Pu was not leached by hot digestion with conc. HNO³ + H₂O₂, indicating the presence of Pu associated with fused silicates. Further, the presence of hot-particles from the Pu contaminants by a-track radiography technique using CR-39 polycarbonate was confirmed in the soil, even at present, after about 50 years from the first nuclear weapon testing. This revised version was published online in July 2006 with corrections to the Cover Date.     

Studies of the vertical distribution of134Cs,137Cs,238Pu,239, 240Pu,241Pu,241Am and210Pb in ombrogenous mires at mid-latitudes

Six peat cores taken from three unmodified blanket and raised bogs in Ireland were sectioned and analyzed for a range of radionuclides including¹³⁴Cs,¹³⁷Cs,²³⁸Pu,²³⁹Pu,²⁴¹Am, and²¹⁰Pb.¹³⁴Cs and¹³⁷Cs were measured by high resolution gamma-spectrometry, while the transuranium nuclides were determined after chemical separation by alpha-spectrometry.²⁴¹Pu, present on the electroplated discs together with Pu(), was measured directly by low-level liquid scintillation counting. Core chronologies were established by measuring the unsupported²¹⁰Pb component using low energy photon spectrometry (LEPS). From the resulting profiles, relaxation depths and migration rates for the above mentioned radionuclides have been determined and differences in the values of these parameters interpreted.²³⁸Pu/^239,240Pu and²⁴¹Pu/^239,240Pu ratios have been examined carefully and are discussed in some detail. Finally, the contribution from Chernobyl to the total radiocaesium inventory in each core has been established using the¹³⁴Cs/¹³⁷Cs ratio observed in the initial fallout from Chernobyl.     

The ambient gamma dose-rate and the inventory of fission products estimations with the soil samples collected at Canadian embassy in Tokyo during Fukushima nuclear accident

In this study, soil samples were collected at Canadian embassy in Tokyo (about 300 km from Fukushima) on 23 March and 23 May of 2011 for purposes of estimating concentrations of radionuclides in fallout, the total fallout inventory, the depth distribution of radionuclide of interest and the elevated ambient gamma dose-rate at this limited location. Some fission products and actinides were analyzed using gamma-ray spectrometry, alpha spectrometry and liquid scintillation counting. The elevated activity concentration levels of ¹³¹I, ¹³²I, ¹³⁴Cs, ¹³⁷Cs, ¹³⁶Cs, ¹³²Te, ¹²⁹mTe, ¹²⁹Te, ¹⁴⁰Ba and ¹⁴⁰La were measured by the gamma-ray spectrometer in the first sample collected on 23 March. Two months after the accident, the ¹³⁴Cs and ¹³⁷Cs became only detectable nuclides. A mass relaxation depth of 3.0 g/cm² was determined by the activities on the depth distribution of ¹³⁷Cs in a soil core. The total fallout inventory was thus calculated as 225 kBq/m² on March sampling date and 25 kBq/m² on May sampling date. The ambient gamma dose-rates in the sampling area estimated by the fallout fission products inventory and ¹³⁷Cs depth distribution ranged from 184 to 38 nGy/h. There was no detectable americium or plutonium in the soil samples by alpha spectrometry. Although ⁹⁰Sr or ⁸⁹Sr were detected supposedly as a result of this accident, it was less than the detection limit, which was about 0.4 Bq/kg in the soil samples.     

Determination of137Cs and134Cs radioisotopes in various mushrooms from Austria one year after the Chernobyl incident

Many mushrooms from Austria collected between May 25 and September 21, 1987 were analyzed for¹³⁷Cs and¹³⁴Cs by -spectroscopy one year after the reactor accident at Chernobyl. The following concentrations /nCi kg^–1 wet weight/ were found:¹³⁷Cs 0.4–43.2 nCi kg^–1,¹³⁴Cs 0.1–16.4 nCi kg^–1. The concentration of cesium isotopes in Cantharellus cibarius /Klagenfurt/ and Xerocomus badius /Upper-Austria, Mühlviertel/ were considerably higher than the tolerance level /5 nCi kg^–1/.     

Distribution of 137Cs and 134Cs in the North Pacific Ocean: impacts of the TEPCO Fukushima-Daiichi NPP accident

Impact of the TEPCO Fukushima-Daiichi NPP accident, FNPP1, to the North Pacific Ocean occurred through two pathways, namely direct release and atmospheric deposition to wide ocean surface. We collected more than 100 seawater samples in the North Pacific Ocean in April and May 2011 by seven commercial ships as VOS. Since the sample volume was 2 l each, we measured radiocaesium activity at Ogoya Underground Facility to obtain reliable activity. ¹³⁷Cs was detected at all stations and ¹³⁴Cs was detected at most of the stations in the North Pacific Ocean. The ¹³⁷Cs activity ranged from around 1 to 1,000 Bq m^?3 with activity ratios of ¹³⁴Cs/¹³⁷Cs close to 1 which is a signature of radiocaesium originated from the FNPP1 accident. At east of the International Date Line north of 40°N in the Pacific Ocean in April 2011, the ¹³⁴Cs activity ranged from 2 to 12 Bq m^?3.