Amendments to (63)Ni production calculation for Hiroshima by Takamiya et al. and DS02 fluence data by Egbert et al.

In a previous paper, Takamiya et al. calculated (63)Ni production in copper samples exposed to the Hiroshima atomic bomb. More specifically, they used their experimental cross-section values of the (63)Cu(n,p)(63)Ni reaction and compared the result with that of the corresponding calculation in the radiation dosimetry system DS02, which used another set of cross-section values. These results were different, and the following two reasons were found: typographical errors in several energy boundary values in the DS02 report that was also used in the calculation by Takamiya et al. and an inappropriate assumption on the cross-section values of the low neutron energy region in the calculation by Takamiya et al. These two issues are described and amended in the present report.

Measuring fast neutrons in Hiroshima at distances relevant to atomic-bomb survivors.

Data from the survivors of the atomic bombs serve as the major basis for risk calculations of radiation-induced cancer in humans. A controversy has existed for almost two decades, however, concerning the possibility that neutron doses in Hiroshima may have been much larger than estimated. This controversy was based on measurements of radioisotopes activated by thermal neutrons that suggested much higher fluences at larger distances than expected. For fast neutrons, which contributed almost all the neutron dose, clear measurement validation has so far proved impossible at the large distances (900 to 1,500 m) most relevant to survivor locations. Here, the first results are reported for the detection of 63Ni produced predominantly by fast neutrons (above about 1 MeV) in copper samples from Hiroshima. This breakthrough was made possible by the development of chemical extraction methods and major improvements in the sensitivity of accelerator mass spectrometry for detection of 63Ni atoms (refs 8-11). When results are compared with 63Ni activation predicted by neutron doses for Hiroshima survivors, good agreement is observed at the distances most relevant to survivor data. These findings provide, for the first time, clear measurement validation of the neutron doses to survivors in Hiroshima.

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.

Atomic bomb induced 152Eu: reconciliation of discrepancy between measurements and calculation.

In order to resolve the discrepancy between the measured and calculated 152Eu activity induced by the atomic bomb at Hiroshima, extremely low background gamma-ray spectrometry was performed for 17 granite samples collected from 134 m to more than 3 km from the hypocenter. Measurements agreed well with theoretical calculations based on DS02 up to 1.4 km from hypocenter.

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.

DS02R1: Improvements to Atomic Bomb Survivors' Input Data and Implementation of Dosimetry System 2002 (DS02) and Resulting Changes in Estimated Doses.

Individual dose estimates calculated by Dosimetry System 2002 (DS02) for the Life Span Study (LSS) of atomic bomb survivors are based on input data that specify location and shielding at the time of the bombing (ATB). A multi-year effort to improve information on survivors' locations ATB has recently been completed, along with comprehensive improvements in their terrain shielding input data and several improvements to computational algorithms used in combination with DS02 at RERF. Improvements began with a thorough review and prioritization of original questionnaire data on location and shielding that were taken from survivors or their proxies in the period 1949-1963. Related source documents varied in level of detail, from relatively simple lists to carefully-constructed technical drawings of structural and other shielding and surrounding neighborhoods. Systematic errors were reduced in this work by restoring the original precision of map coordinates that had been truncated due to limitations in early data processing equipment and by correcting distortions in the old (WWII-era) maps originally used to specify survivors' positions, among other improvements. Distortion errors were corrected by aligning the old maps and neighborhood drawings to orthophotographic mosaics of the cities that were newly constructed from pre-bombing aerial photographs. Random errors that were reduced included simple transcription errors and mistakes in identifying survivors' locations on the old maps. Terrain shielding input data that had been originally estimated for limited groups of survivors using older methods and data sources were completely re-estimated for all survivors using new digital terrain elevation data. Improvements to algorithms included a fix to an error in the DS02 code for coupling house and terrain shielding, a correction for elevation at the survivor's location in calculating angles to the horizon used for terrain shielding input, an improved method for truncating high dose estimates to 4 Gy to reduce the effect of dose error, and improved methods for calculating averaged shielding transmission factors that are used to calculate doses for survivors without detailed shielding input data. Input data changes are summarized and described here in some detail, along with the resulting changes in dose estimates and a simple description of changes in risk estimates for solid cancer mortality. This and future RERF publications will refer to the new dose estimates described herein as "DS02R1 doses."

Neutrons confirmed in Nagasaki and at the Army Pulsed Radiation Facility: implications for Hiroshima.

Recent reports have clearly demonstrated that large discrepancies exist between neutron activation measured in Hiroshima and activation calculated using the current dosimetry system, DS86. The reports confirmed previous results for cobalt activation in Hiroshima that suggested problems, and this has spurred a joint U.S.-Japan effort to identify the source(s) of this discrepancy. Here, new results are presented that appear to eliminate both the measurements of neutron activation and the DS86 air-transport calculations as potential sources of the discrepancy in Hiroshima. Computer transport of DS86 fission neutrons through large distances of air was validated using concrete samples from Nagasaki and chloride detectors placed at selected distances from a bare uranium reactor. In both cases, accelerator mass spectrometry was used to measure thermal neutron activation via the reaction, 35Cl(n, gamma)36Cl (half-life, 301,000 years). Good agreement was observed between measurements of neutron activation and DS86 calculations for Nagasaki, as well as for the reactor experiment. Thus the large discrepancy observed in Hiroshima appears not to be due to uncertainties in air-transport calculations or in the activation measurements; rather, the discrepancy appears to be due to uncertainties associated with the Hiroshima bomb itself.

A spectral unfolding method to determine source depth distribution.

The depth distribution in tissue of a gamma-emitting isotope can be estimated by observing the energy spectrum of photons emerging from the body. Monte Carlo methods were used to compute surface energy spectra for 99Tcm point sources at various depths. From these noise-free results a discrete response matrix was constructed to relate the input source depth to the corresponding output spectrum. Observed spectra with noise were then simulated independently by Monte Carlo calculations assuming various measurement times and source strengths. The source distribution was determined by solving the discrete inverse unfolding problem by the Method of Regularisation. The effective depth resolution is seen to depend strongly upon measurement time. The results show that limited depth resolution can be obtained from a single view of the object region.

Neutron discrepancies in the DS86 Hiroshima dosimetry system.

More than a decade has passed since a complete revision was initiated of the radiation doses received by survivors of the Hiroshima and Nagasaki atomic bombings. The new dosimetry system (DS86) was completed in 1986 and adopted shortly thereafter. Overall, DS86 was noted to be a clear improvement over the old dosimetry system. However, based on limited validation measurements, troublesome inconsistencies were suggested for neutrons. Since 1986, a substantial number of additional neutron activation measurements have been made in mineral and metal samples from Hiroshima. Importantly, a large number of measurements have now been made at distances beyond 1 km. Here, inconsistencies between neutron activation measurements and DS86 calculations for Hiroshima are examined using all available measurement data, including new measurements for 36Cl which extend the measurement range to more than 1.7 km from the epicenter, and Monte Carlo modeling calculations for each sample measured. Results show that thermal neutron activation measured beyond approximately 1 km in Hiroshima (at distances most relevant for radiation-risk evaluation) is two to 10, or more, times higher than that calculated based on DS86. Similar trends observed when comparing results by several independent measurement laboratories, using different analytical methods, suggest that the DS86 calculations for low-energy neutrons are in error. Because of the importance of the Hiroshima data in radiation risk evaluation, this large discrepancy is in need of resolution.

(41)Ca in Tooth Enamel. Part II: A means for retrospective biological neutron dosimetry in atomic bomb survivors.

(41)Ca is produced mainly by absorption of low-energy neutrons on stable (40)Ca. We used accelerator mass spectrometry (AMS) to measure (41)Ca in enamel of 16 teeth from 13 atomic bomb survivors who were exposed to the bomb within 1.2 km from the hypocenter in Hiroshima. In our accompanying paper (Wallner et al., Radiat. Res. 174, 000-000, 2010), we reported that the background-corrected (41)Ca/Ca ratio decreased from 19.5 x 10(-15) to 2.8 x 10(-15) with increasing distance from the hypocenter. Here we show that the measured ratios are in good correlation with gamma-ray doses assessed by electron paramagnetic resonance (EPR) in the same enamel samples, and agree well with calculated ratios based on either the current Dosimetry System 2002 (DS02) or more customized dose estimates where the regression slope as obtained from an errors-in-variables linear model was about 0.85. The calculated DS02 neutron dose to the survivors was about 10 to 80 mGy. The low-energy neutrons responsible for (41)Ca activation contributed variably to the total neutron dose depending on the shielding conditions. Namely, the contribution was smaller (10%) when shielding conditions were lighter (e.g., outside far away from a single house) and was larger (26%) when they were heavier (e.g., in or close to several houses) because of local moderation of neutrons by shielding materials. We conclude that AMS is useful for verifying calculated neutron doses under mixed exposure conditions with gamma rays.

Structure determination of adsorbed hydrogen on a real catalyst.

Here we show that neutron diffraction can experimentally measure distances involving hydrogen on real catalysts. This method is applicable to adsorbed hydrogen (and other hydrogenous species) on crystalline, nanocrystalline or amorphous materials, supported and unsupported metals as well as oxides and works at ambient temperature and pressure.

Intercomparison study on (152)Eu gamma ray and (36)Cl AMS measurements for development of the new Hiroshima-Nagasaki Atomic Bomb Dosimetry System 2002 (DS02).

In the process of developing a new dosimetry system for atomic bomb survivors in Hiroshima and Nagasaki (DS02), an intercomparison study between (152)Eu and (36)Cl measurements was proposed, to reconcile the discrepancy previously observed in the Hiroshima data between measurements and calculations of thermal neutron activation products. Nine granite samples, exposed to the atomic-bomb radiation in Hiroshima within 1,200 m of the hypocenter, as well as mixed standard solutions containing known amounts of europium and chlorine that were neutron-activated by a (252)Cf source, were used for the intercomparison. Gamma-ray spectrometry for (152)Eu was carried out with ultra low-background Ge detectors at the Ogoya Underground Laboratory, Kanazawa University, while three laboratories participated in the (36)Cl measurement using accelerator mass spectrometry (AMS): The Technical University of Munich, Germany, the Lawrence Livermore National Laboratory, USA and the University of Tsukuba, Japan. Measured values for the mixed standard solutions showed good agreement among the participant laboratories. They also agreed well with activation calculations, using the neutron fluences monitored during the (252)Cf irradiation, and the corresponding activation cross-sections taken from the JENDL-3.3 library. The measured-to-calculated ratios obtained were 1.02 for (152)Eu and 0.91-1.02 for (36)Cl, respectively. Similarly, the results of the granite intercomparison indicated good agreement with the DS02 calculation for these samples. An average measured-to-calculated ratio of 0.98 was obtained for all granite intercomparison measurements. The so-called neutron discrepancy that was previously observed and that which included increasing measured-to-calculated ratios for thermal neutron activation products for increasing distances beyond 1,000 m from the hypocenter was not seen in the results of the intercomparison study. The previously claimed discrepancy could be explained by insufficient understanding of the measured data.

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.

36Cl measurements in Hiroshima granite samples as part of an international intercomparison study. Results from the Munich group.

Within the effort to resolve the so-called Hiroshima neutron discrepancy, an international intercomparison study has been carried out on granite samples from Hiroshima, with participating institutions from Japan, the US, and Germany. (36)Cl and (152)Eu produced in these samples by thermal neutrons from the A-bomb explosion were assessed independently by means of different techniques. At the Maier-Leibnitz-Laboratory near Munich, Germany, (36)Cl concentrations were measured by accelerator mass spectrometry. Measured (36)Cl/Cl ratios ranged from 1,670 x 10(-13) (at a distance of 146 m from the hypocenter) to 2.2 x 10(-13) (at a distance of 1,163 m from the hypocenter). One granite sample not exposed to A-bomb neutrons was measured as a control, and a (36)Cl/Cl ratio of 2.6 x 10(-13) was obtained. On average, our experimental results are 20-30% lower than those provided by model calculations based on the dosimetry system DS86. The results presented here do not support previous assessments of (36)Cl, (60)Co, and (152)Eu which had suggested much larger thermal neutron fluences than those calculated on the basis of DS86 for distances from the hypocenter of more than 1,000 m.