Distribution of 60Co in steel samples from Hiroshima.

This paper describes ultra low-level gamma-ray spectrometry measurements of the (60)Co activity distribution inside one 52 mm and one 41 mm thick steel sample. The samples had been exposed to the Hiroshima atomic bomb and were from the Aioi bridge and the Yokogawa bridge. Both samples were measured in a recent study aiming to back up model calculation of Hiroshima dosimetry. The (60)Co activity distributions found in this study support the assumptions made in the previous study.

Measurement of soil contamination by radionuclides due to the Fukushima Dai-ichi Nuclear Power Plant accident and associated estimated cumulative external dose estimation.

Soil sampling was carried out at an early stage of the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. Samples were taken from areas around FDNPP, at four locations northwest of FDNPP, at four schools and in four cities, including Fukushima City. Radioactive contaminants in soil samples were identified and measured by using a Ge detector and included (129 m)Te, (129)Te, (131)I, (132)Te, (132)I, (134)Cs, (136)Cs, (137)Cs, (140)Ba and (140)La. The highest soil depositions were measured to the northwest of FDNPP. From this soil deposition data, variations in dose rates over time and the cumulative external doses at the locations for 3 months and 1y after deposition were estimated. At locations northwest of FDNPP, the external dose rate at 3 months after deposition was 4.8-98 µSv/h and the cumulative dose for 1 y was 51 to 1.0 × 10(3)mSv; the highest values were at Futaba Yamada. At the four schools, which were used as evacuation shelters, and in the four urban cities, the external dose rate at 3 months after deposition ranged from 0.03 to 3.8µSv/h and the cumulative doses for 1 y ranged from 3 to 40 mSv. The cumulative dose at Fukushima Niihama Park was estimated as the highest in the four cities. The estimated external dose rates and cumulative doses show that careful countermeasures and remediation will be needed as a result of the accident, and detailed measurements of radionuclide deposition densities in soil will be important input data to conduct these activities.

Fast neutrons measured in copper from the Hiroshima atomic bomb dome.

The first measurements of (63)Ni produced by A-bomb fast neutrons (above approximately 1 MeV) in copper samples from Hiroshima encompassed distances from approximately 380 to 5062 m from the hypocenter (the point on the ground directly under the bomb). They included the region of interest to survivor studies (approximately 900 to 1500 m) and provided the first direct validation of fast neutrons in that range. However, a significant measurement gap remained between the hypocenter and 380 m. Measurements close to the hypocenter are important as a high-value anchor for the slope of the curve for neutron activation as a function of distance. Here we report measurements of (63)Ni in copper samples from the historic Hiroshima Atomic Bomb Dome, which is located approximately 150 m from the hypocenter. These measurements extend the range of our previously published data for (63)Ni providing a more comprehensive and consistent A-bomb activation curve. The results are also in good agreement with calculations based on the current dosimetry system (DS02) and give further experimental support to the accuracy of this system that forms the basis for radiation risk estimates worldwide.

Radioactivity in atomic-bomb samples from exposure to environmental neutrons.

For about one decade, activation measurements performed on environmental samples from a distance larger than 1 km from the hypocenter of the atomic-bomb explosion over Hiroshima suggested much higher thermal neutron fluences to the survivors than predicted. This caused concern among the radiation protection community and prompted a complete re-evaluation of all aspects of survivor dosimetry. While it was shown recently that secondary neutrons from cosmic radiation and other sources have probably been the reason for the high measured concentrations of the long-lived radioisotope 36Cl in these samples, the source for high measured concentrations of the short-lived radionuclides 152Eu and 60Co has not yet been investigated in detail. In order to quantify the production of 152Eu and 60Co in environmental samples by secondary neutrons from cosmic radiation, thermal neutron fluxes were measured by means of a He gas proportional counter in various buildings where these samples had been and still are being stored. Because a 252Cf neutron source has been operated occasionally close to one of the sample storage rooms, additional neutron flux measurements were carried out when the neutron source was in operation. The thermal neutron fluxes measured ranged from 0.00017 to 0.00093 n cm(-2) s(-1) and depended on the floor number of the investigated building. Based on the measured neutron fluxes, the specific activities from the reactions 151Eu(n,gamma)152Eu and 59Co(n,gamma)60Co in the atomic-bomb samples were estimated to be 7.9 mBq g(-1) Eu and 0.27 mBq g(-1) Co, respectively, in saturation. These activities are much lower than those recently measured in samples that had been exposed to atomic-bomb neutrons. It is therefore concluded that environmental and moderated 252Cf neutrons are not the source for the high activities that had been measured in these samples.

Neutron-induced 63Ni in copper samples from Hiroshima and Nagasaki: a comprehensive presentation of results obtained at the Munich Maier-Leibnitz Laboratory.

Those inhabitants of Hiroshima and Nagasaki who were affected by the A-bomb explosions, were exposed to a mixed neutron and gamma radiation field. Few years later about 120,000 survivors of both cities were selected, and since then radiation-induced late effects such as leukemia and solid tumors are being investigated in this cohort. When the present study was initiated, the fast neutron fluences that caused the neutron doses of these survivors had never been determined experimentally. In principle, this would have been possible if radioisotopes produced by fast neutrons from the A-bomb explosions had been detected in samples from Hiroshima and Nagasaki at distances where the inhabitants survived. However, no suitable radioisotope had so far been identified. As a contribution to a large international effort to re-evaluate the A-bomb dosimetry, the concentration of the radionuclide (63)Ni (half-life 100.1 years) has been measured in copper samples from Hiroshima and Nagasaki. These measurements were mainly performed at the Maier-Leibnitz-Laboratory in Munich, Germany, by means of accelerator mass spectrometry. Because the (63)Ni had been produced in these samples by fast A-bomb neutrons via the reaction (63)Cu(n,p)(63)Ni, these measurements allow direct experimental validation of calculated neutron doses to the members of the LSS cohort, for the first time. The results of these efforts have already been published in a compact form. A more detailed discussion of the methodical aspects of these measurements and their results are given in the present paper. Eight copper samples that had been significantly exposed to fast neutrons from the Hiroshima A-bomb explosion were investigated. In general, measured (63)Ni concentrations decreased in these samples with increasing distance to the hypocenter, from 4 x 10(6 ) (63)Ni nuclei per gram copper at 391 m, to about 1 x 10(5 ) (63)Ni nuclei per gram copper at about 1,400 m. Additional measurements performed on three large-distant copper samples from Hiroshima (distance to the hypocenter 1,880-7,500 m) and on three large-distant copper samples from Nagasaki (distance to the hypocenter 3,931-4,428 m) that were not exposed significantly to A-bomb neutrons, suggest a typical background concentration of about 8 x 10(4 ) (63)Ni nuclei per gram copper. If the observed background is accounted for, the results are consistent with state-of-the-art neutron transport calculations for Hiroshima, in particular for those distances where the victims survived and were included in the life span study cohort.

Microdosimetry of neutron field for boron neutron capture therapy at Kyoto university reactor.

Microdosimetric single event spectrum in a human body simulated by an acrylic phantom has been measured for the clinical BNCT field at the Kyoto University Reactor (KUR). The recoil particles resulting from the initial reaction and subsequent interactions, namely protons, electrons, alpha particles and carbon nuclei are identified in the microdosimetric spectrum. The relative contributions to the neutron dose from proton, alpha particles and carbon are estimated to be about 0.9, 0.07 and 0.3, respectively, four depths between 5 and 41 mm. We estimate that the dose averaged lineal energy, yD decreased with depth from 64 to 46 keV microm(-1). Relative biological effectiveness (RBE) of this neutron field using a response function for the microdosimetric spectrum was estimated to decrease from 3.6 to 2.9 with increasing depth.

Characterisation of an ultra-miniature counter for microdosimetric measurements in a therapeutic 400 MeV/A carbon beam.

Single event spectra of a clinical carbon beam have been measured by an ultra-miniature tissue-equivalent proportional counter (UMC). In order to cover the energy range of the Bragg peak, the incident energy of the carbon beam was degraded by aluminium plates. Single event spectra for carbon-events incident to the UMC were analysed and selected at several carbon energies using thin scintillation counters. It was found that the dose weighted lineal energy distributions have a doublet peak structure due to incident carbon beam and fragment contributions.

Calculation of the neutron W value for neutron dosimetry below the MeV energy region.

The effective neutron W value for tissue-equivalent gas in the energy region from 5 keV to 5.7 MeV has been calculated using W values for recoil particles (protons, alpha particles, oxygen, carbon and nitrogen ions), which are produced by incident neutrons. The W value is assumed to be an energy-fluence-average over the W values of the recoil particles. The energy fluence spectra for the recoil particles are calculated by using a continuous slowing down approximation (CSDA). For the W values of recoil particles in the low-energy region, the recently evaluated data by Siebert et al and Taylor et al were used. Results are presented which show that the effective neutron W value depends strongly on energy in the low-energy region. This result indicates that neutron dose measurements using ionization chambers need a considerable correction of the W value in the low-energy region.

DS86 neutron dose: Monte Carlo analysis for depth profile of 152Eu activity in a large stone sample.

The depth profile of 152Eu activity induced in a large granite stone pillar by Hiroshima atomic bomb neutrons was calculated by a Monte Carlo N-Particle Transport Code (MCNP). The pillar was on the Motoyasu Bridge, located at a distance of 132 m (WSW) from the hypocenter. It was a square column with a horizontal sectional size of 82.5 cm x 82.5 cm and height of 179 cm. Twenty-one cells from the north to south surface at the central height of the column were specified for the calculation and 152Eu activities for each cell were calculated. The incident neutron spectrum was assumed to be the angular fluence data of the Dosimetry System 1986 (DS86). The angular dependence of the spectrum was taken into account by dividing the whole solid angle into twenty-six directions. The calculated depth profile of specific activity did not agree with the measured profile. A discrepancy was found in the absolute values at each depth with a mean multiplication factor of 0.58 and also in the shape of the relative profile. The results indicated that a reassessment of the neutron energy spectrum in DS86 is required for correct dose estimation.

A method to detect low-level 63Ni activity for estimating fast neutron fluence from the Hiroshima atomic bomb.

The Hiroshima and Nagasaki atomic bombs resulted in the worst reported exposure of radiation to the human body. The data of survivors have provided the basis for the risk estimation for ionizing radiation, and thus are widely used as the basis of radiation safety. In this report we have studied a new method to detect the low-level 63Ni activity in copper samples in order to estimate the fast neutron fluence from the Hiroshima atomic bomb. Only 0.8 x 10(-3) Bq g(-1) of 63Ni is expected to be produced by the atomic bomb in a copper sample with the 63Cu(n, p)63Ni reaction at a distance of 500 m from the hypocenter. Our method has the required level of sensitivity for determination of the fast neutron fluence out to distances of at least 500 m, and perhaps as far as 1,000 m. We have already investigated and collected some bomb-irradiated copper samples for further study.

Uncertainties of DS86 and prospects for residual radioactivity measurement.

Residual radioactivity data of 152Eu, 60Co and 36Cl have been accumulated and it has been revealed in the thermal neutron region that a systematic discrepancy exists between the measured data and activation calculation based on the DS86 neutrons in Hiroshima. Recently 63Ni produced in copper samples by the fast neutron reaction 63Cu(n,p)63Ni has been of interest for evaluation of fast neutrons. Reevaluation of atomic-bomb neutrons and prospects based on residual activity measurements have been discussed.

A crack model of the Hiroshima atomic bomb: explanation of the contradiction of "Dosimetry system 1986".

There has been a large discrepancy between the Dosimetry system 1986 (DS86) and measured data, some of which data in Hiroshima at about 1.5 km ground distance from the hypocenter are about 10 times larger than the calculation. Therefore its causes have long been discussed, since it will change the estimated radiation risks obtained based on the Hiroshima and Nagasaki data. In this study the contradiction was explained by a bare-fission-neutron leakage model through a crack formed at the time of neutron emission. According to the present calculation, the crack has a 3 cm parallel spacing, which is symmetric with respect to the polar axis from the hypocenter to the epicenter of the atomic bomb. We made also an asymmetric opening closing 3/4 of this symmetric geometry, because there are some data which shows asymmetry. In addition, the height of the neutron emission point was elevated 90 m. By using the asymmetric calculation, especially for long distant data located more than 1 km, it was verified that all of the activity data induced by thermal and fast neutrons, were simultaneously explained within the data scattering. The neutron kerma at a typical 1.5 km ground distance increases 3 and 8 times more than DS86 based on the symmetric and asymmetric model, respectively.

Residual 60Co activity in steel samples exposed to the Hiroshima atomic-bomb neutrons.

Residual 60Co radioactivity produced by the neutrons from the Hiroshima atomic bomb has been measured by means of gamma-ray spectrometry for seven steel samples located up to 1,800 m slant range and one control sample obtained at 4.5 km from the hypocenter. After removing the main constituent of iron ions from the steel sample by the solvent extraction method, nickel and cobalt were chemically separated by the ion exchange process. Gamma-ray measurements were performed with a low background well-type germanium detector. Derived specific activities 60Co:Co were compared with previous measurements and with the calculation based on the neutron fluence of current dosimetry system DS86. It has been shown that a systematic discrepancy exists between the measured and calculated activity. The calculated-to-measured ratios for 60Co are consistent with those of 152Eu and 36Cl activity.

152Eu depth profiles in granite and concrete cores exposed to the Hiroshima atomic bomb.

Two granite and two concrete core samples were obtained within 500 m from the hypocenter of the Hiroshima atomic bomb, and the depth profile of 152Eu was measured to evaluate the incident neutron spectrum. The granite cores were obtained from a pillar of the Motoyasu Bridge located 101 m from the hypocenter and from a granite rock in the Shirakami Shrine (379 m); the concrete cores were obtained from a gate in the Gokoku Shrine (398 m) and from a pillar top of the Hiroshima bank (250 m). The profiles of the specific activities of the cores were measured to a depth of 40 cm from the surface using low background germanium (Ge) spectrometers. According to the measured depth profiles, relaxation lengths of incident neutrons were derived as 13.6 cm for Motoyasu Bridge pillar (granite), 12.2 cm for Shirakami Shrine core (granite), and 9.6 cm for concrete cores of Gokoku Shrine and Hiroshima Bank. In addition, a comparison of the granite cores in Hiroshima showed good agreement with Nagasaki data. Present results indicates that the depth profile of 152Eu reflects incident neutrons not so high but in the epithermal region.

137Cs concentration in soil samples from an early survey of Hiroshima atomic bomb and cumulative dose estimation from the fallout.

Low background gamma-ray measurement has been performed to determine the 137Cs content in soil samples collected in a very early survey of the Hiroshima atomic bomb. These soil samples were collected just 3 d after the explosion within 5 km from the hypocenter and were not exposed to the global fallout from nuclear weapon tests. Out of 22 samples, 137Cs was detected for 11 samples, and their radioactivities ranged from 0.16-10.6 mBq g-1 at the time of the measurement. A comparison of the 137Cs deposition with the rainfall area within Hiroshima city indicates that the rainfall area was wider than the previously proposed one. Cumulative exposure by the fallout has been estimated to be 0.31 mC kg-1 (0.12 R) in Hiroshima city except for the heavy fallout area and at most 1.0 mC kg-1 (4 R) in the heavy fallout area.

Benchmark test of neutron transport calculations: indium, nickel, gold, europium, and cobalt activation with and without energy moderated fission neutrons by iron simulating the Hiroshima atomic bomb casing.

A benchmark test of the Monte Carlo neutron and photon transport code system (MCNP) was performed using a bare- and energy-moderated 252Cf fission neutron source which was obtained by transmission through 10-cm-thick iron. An iron plate was used to simulate the effect of the Hiroshima atomic bomb casing. This test includes the activation of indium and nickel for fast neutrons and gold, europium, and cobalt for thermal and epithermal neutrons, which were inserted in the moderators. The latter two activations are also to validate 152Eu and 60Co activity data obtained from the atomic bomb-exposed specimens collected at Hiroshima and Nagasaki, Japan. The neutron moderators used were Lucite and Nylon 6 and the total thickness of each moderator was 60 cm or 65 cm. Measured activity data (reaction yield) of the neutron-irradiated detectors in these moderators decreased to about 1/1,000th or 1/10,000th, which corresponds to about 1,500 m ground distance from the hypocenter in Hiroshima. For all of the indium, nickel, and gold activity data, the measured and calculated values agreed within 25%, and the corresponding values for europium and cobalt were within 40%. From this study, the MCNP code was found to be accurate enough for the bare- and energy-moderated 252Cf neutron activation calculations of these elements using moderators containing hydrogen, carbon, nitrogen, and oxygen.

Residual 152Eu and 60Co activities induced by neutrons from the Hiroshima atomic bomb.

Specific activities of 152Eu:Eu in stone samples exposed to the Hiroshima atomic bomb were determined for 70 samples up to a 1,500-m slant range from the epicenter. The specific activities of 60Co:Co were also determined for six samples near the Hiroshima hypocenter. First, the 152Eu data were investigated to find out the directional dependence of neutron activation. Directional anisotropy was not definite; however, there was an indication that the activation in the west-southwest was lower than in other directions. Second, measured 152Eu and 60Co radioactivity data were compared with activation calculations based on DS86 neutrons. It is clearly shown that the measured data are lower than the calculation near the hypocenter and vice versa at long distances beyond 1,000 m. The calculated-to-measured ratios of 152Eu are 1.6 at the hypocenter, 1.0 at approximately 900 m, and 0.05 at a 1,500-m slant range. Present results indicate that systematic errors exist in the DS86 neutrons concerning the source-term spectrum, neutron transport calculations in air, and/or activation measurements.

Benchmark test of transport calculations of gold and nickel activation with implications for neutron kerma at Hiroshima.

A benchmark test of the Monte Carlo neutron and photon transport code system (MCNP) was performed using a 252Cf fission neutron source to validate the use of the code for the energy spectrum analyses of Hiroshima atomic bomb neutrons. Nuclear data libraries used in the Monte Carlo neutron and photon transport code calculation were ENDF/B-III, ENDF/B-IV, LASL-SUB, and ENDL-73. The neutron moderators used were granite (the main component of which is SiO2, with a small fraction of hydrogen), Newlight [polyethylene with 3.7% boron (natural)], ammonium chloride (NH4Cl), and water (H2O). Each moderator was 65 cm thick. The neutron detectors were gold and nickel foils, which were used to detect thermal and epithermal neutrons (4.9 eV) and fast neutrons (> 0.5 MeV), respectively. Measured activity data from neutron-irradiated gold and nickel foils in these moderators decreased to about 1/1,000th or 1/10,000th, which correspond to about 1,500 m ground distance from the hypocenter in Hiroshima. For both gold and nickel detectors, the measured activities and the calculated values agreed within 10%. The slopes of the depth-yield relations in each moderator, except granite, were similar for neutrons detected by the gold and nickel foils. From the results of these studies, the Monte Carlo neutron and photon transport code was verified to be accurate enough for use with the elements hydrogen, carbon, nitrogen, oxygen, silicon, chlorine, and cadmium, and for the incident 252Cf fission spectrum neutrons.

Specific activities of 60Co and 152Eu in samples collected from the Atomic-Bomb Dome in Hiroshima.

Neutron-induced activities 60Co and 152Eu have been measured for samples collected from the Atomic-Bomb Dome locating at 161 m from the hypocenter of the Hiroshima Bomb. Specific activities 60Co/Co and 152Eu/Eu at the time of the detonation have been determined as 10.0 +/- 1.0 Bq mg-1 (steel sample S4) and 80 +/- 9 Bq mg-1 (granite sample G1), respectively. Detailed measurements of 60Co and 152Eu activities for samples collected from various locations of the Dome show almost no directional dependence whether the sample faced to the epicenter or not, nor vertical height dependence between 17 m height and the ground level. In addition, 152Eu was not detected in the sample collected from the basement. It has been shown that the present 60Co activity value, the nearest steel one to the hypocenter, as well as other short distance data are systematically lower than the calculated values based on the neutron fluence of the DS86.