Shape Coexistence at Zero Spin in

The low-spin structure of the semimagic ^{64}Ni nucleus has been considerably expanded: combining four experiments, several 0^{+} and 2^{+} excited states were identified below 4.5 MeV, and their properties established. The Monte Carlo shell model accounts for the results and unveils an unexpectedly complex landscape of coexisting shapes: a prolate 0^{+} excitation is located at a surprisingly high energy (3463 keV), with a collective 2^{+} state 286 keV above it, the first such observation in Ni isotopes. The evolution in excitation energy of the prolate minimum across the neutron N=40 subshell gap highlights the impact of the monopole interaction and its variation in strength with N.

Supernova-Produced

For the time period from 1.5 to 4 Myr before the present we found in deep ocean ferromanganese crusts a ^{53}Mn excess concentration in terms of ^{53}Mn/Mn of about 4×10^{-14} over that expected for cosmogenic production. We conclude that this ^{53}Mn is of supernova origin because it is detected in the same time window, about 2.5 Myr ago, where ^{60}Fe has been found earlier. This overabundance confirms the supernova origin of that ^{60}Fe. For the first time, supernova-formed ^{53}Mn has been detected and it is the second positively identified radioisotope from the same supernova. The ratio ^{53}Mn/^{60}Fe of about 14 is consistent with that expected for a SN with a 11-25 M_{⊙} progenitor mass and solar metallicity.

Interstellar

A dying massive star ends in a supernova explosion ejecting a large fraction of its mass into the interstellar medium. If this happens nearby, part of the ejecta might end on Solar System bodies and, in fact, radioactive ^{60}Fe has been detected on the Pacific ocean floor in about 2 Ma old layers. Here, we report on the detection of this isotope also in lunar samples, originating presumably from the same event. The concentration of the cosmic ray produced isotope ^{53}Mn, measured in the same samples, proves the supernova origin of the ^{60}Fe. From the ^{60}Fe concentrations found we deduce a reliable value for the local interstellar fluence in the range of 1×10^{8} at/cm^{2}. Thus, we obtain constraints on the recent and nearby supernova(e).

Abundance of live ²44Pu in deep-sea reservoirs on Earth points to rarity of actinide nucleosynthesis.

Half of the heavy elements including all actinides are produced in r-process nucleosynthesis, whose sites and history remain a mystery. If continuously produced, the Interstellar Medium is expected to build-up a quasi-steady state of abundances of short-lived nuclides (with half-lives ≤100 My), including actinides produced in r-process nucleosynthesis. Their existence in today's interstellar medium would serve as a radioactive clock and would establish that their production was recent. In particular (244)Pu, a radioactive actinide nuclide (half-life=81 My), can place strong constraints on recent r-process frequency and production yield. Here we report the detection of live interstellar (244)Pu, archived in Earth's deep-sea floor during the last 25 My, at abundances lower than expected from continuous production in the Galaxy by about 2 orders of magnitude. This large discrepancy may signal a rarity of actinide r-process nucleosynthesis sites, compatible with neutron-star mergers or with a small subset of actinide-producing supernovae.

(41)Ca in tooth enamel. Part I: a biological signature of neutron exposure in atomic bomb survivors.

The detection of (41)Ca atoms in tooth enamel using accelerator mass spectrometry is suggested as a method capable of reconstructing thermal neutron exposures from atomic bomb survivors in Hiroshima and Nagasaki. In general, (41)Ca atoms are produced via thermal neutron capture by stable (40)Ca. Thus any (41)Ca atoms present in the tooth enamel of the survivors would be due to neutron exposure from both natural sources and radiation from the bomb. Tooth samples from five survivors in a control group with negligible neutron exposure were used to investigate the natural (41)Ca content in tooth enamel, and 16 tooth samples from 13 survivors were used to estimate bomb-related neutron exposure. The results showed that the mean (41)Ca/Ca isotope ratio was (0.17 +/- 0.05) x 10(-14) in the control samples and increased to 2 x 10(-14) for survivors who were proximally exposed to the bomb. The (41)Ca/Ca ratios showed an inverse correlation with distance from the hypocenter at the time of the bombing, similar to values that have been derived from theoretical free-in-air thermal-neutron transport calculations. Given that gamma-ray doses were determined earlier for the same tooth samples by means of electron spin resonance (ESR, or electron paramagnetic resonance, EPR), these results can serve to validate neutron exposures that were calculated individually for the survivors but that had to incorporate a number of assumptions (e.g. shielding conditions for the survivors).

(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.

New Measurement of the 60Fe Half-Life.

We have made a new determination of the half-life of the radioactive isotope 60Fe using high precision measurements of the number of 60Fe atoms and their activity in a sample containing over 10(15) 60Fe atoms. Our new value for the half-life of 60Fe is (2.62+/-0.04) x 10(6) yr, significantly above the previously reported value of (1.49+/-0.27) x 10(6) yr. Our new measurement for the lifetime of 60Fe has significant implications for interpretations of galactic nucleosynthesis, for determinations of formation time scales of solids in the early Solar System, and for the interpretation of live 60Fe measurements from supernova-ejecta deposits on Earth.

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.

Search for supernova-produced 60Fe in a marine sediment.

An 60Fe peak in a deep-sea FeMn crust has been interpreted as due to the signature left by the ejecta of a supernova explosion close to the solar system 2.8+/-0.4 Myr ago [Knie, Phys. Rev. Lett. 93, 171103 (2004)10.1103/PhysRevLett.93.171103]. In an attempt to confirm this interpretation with better time resolution and obtain a more direct flux estimate, we measured 60Fe concentrations along a dated marine sediment. We find no 60Fe peak at the expected level from 1.7 to 3.2 Myr ago. Possible causes for the discrepancy are discussed.

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.

60Fe anomaly in a deep-sea manganese crust and implications for a nearby supernova source.

A nearby supernova (SN) explosion in the past can be confirmed by the detection of radioisotopes on Earth that were produced and ejected by the SN. We have now measured a well resolved time profile of the 60Fe concentration in a deep-sea ferromanganese crust and found a highly significant increase 2.8 Myr ago. The amount of 60Fe is compatible with the deposition of ejecta from a SN at a distance of a few 10 pc. The well defined time of the SN explosion makes it possible to search for plausible correlations with other events in Earth's history.

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.

Accelerator mass spectrometry of 63Ni at the Munich Tandem Laboratory for estimating fast neutron fluences from the Hiroshima atomic bomb.

After the release of the present dosimetry system DS86 in 1987, measurements have shown that DS86 may substantially underestimate thermal neutron fluences at large distances (>1,000 m) from the hypocenter in Hiroshima. This discrepancy casts doubts on the DS86 neutron source term and, consequently, the survivors' estimated neutron doses. However, the doses were caused mainly by fast neutrons. To determine retrospectively fast neutron fluences in Hiroshima, the reaction 63Cu(n, p)63Ni can be used, if adequate copper samples can be found. Measuring 63Ni (half life 100 y) in Hiroshima samples requires a very sensitive technique, such as accelerator mass spectrometry (AMS), because of the relatively small amounts of 63Ni expected (approximately 10(5)-10(6) atoms per gram of copper). Experiments performed at Lawrence Livermore National Laboratory have demonstrated in 1996 that AMS can be used to measure 63Ni in Hiroshima copper samples. Subsequently, a collaboration was established with the Technical University of Munich in view of its potential to perform more sensitive measurements of 63Ni than the Livermore facility and in the interest of interlaboratory validation. This paper presents the progress made at the Munich facility in the measurement of 63Ni by AMS. The Munich accelerator mass spectrometry facility is a combination of a high energy tandem accelerator and a detection system featuring a gas-filled magnet. It is designed for high sensitivity measurements of long-lived radioisotopes. Optimization of the ion source setup has further improved the sensitivity for 63Ni by reducing the background level of the 63Cu isobar interference by about two orders of magnitude. Current background levels correspond to a ratio of 63Ni/Ni<2x10(-14) and suggest that, with adequate copper samples, the assessment of fast neutron fluences in Hiroshima and Nagasaki is possible for ground distances of up to 1500 m, and--under favorable conditions--even beyond. To demonstrate this capability, we have measured successfully 6Ni/Ni ratios as low as (3.5 +/- 0.6) x 10(-13). The latter are, based on DS86, representative of a ratio expected from a typical Hiroshima copper sample at about 1,300-m ground range.

The dosimetry system DS86 and the neutron discrepancy in Hiroshima--historical review, present status, and future options.

The historical development of the dosimetry systems for Hiroshima and Nagasaki is outlined from the time immediately after the A-bomb explosions to the publication of the dosimetry system DS86 in 1987, and the present status of the so-called Hiroshima neutron discrepancy is summarized. Several long-lived radionuclides are discussed with regard to their production by neutrons from the A-bomb explosions. With the exception of 63Ni, these radionuclides have not, up to now, been measured in samples from Hiroshima and Nagasaki. Two of them, 63Ni in copper samples and 39Ar in granite samples, were predominantly produced by fast neutrons. 63Ni can be determined by accelerator mass spectrometry with a gas-filled analyzing magnet. It should be measurable, in the near future, in copper samples up to 1500 m from the hypocenter in Hiroshima. 39Ar can be measured in terms of low-level beta-counting. This should be feasible up to a distance of about 1000 m from the hypocenter. Three radionuclides, 10Be, 14C, and 59Ni, were produced predominantly by thermal neutrons with smaller fractions due to the epithermal and fast neutrons, which contribute increasingly more at larger distances from the hypocenter. State-of-the-art accelerator mass spectrometry is likely to permit the determination of 10Be close to the hypocenter and of 14C up to a distance of about 1000 m. 59Ni should be detectable up to a distance of about 1000 m in terms of accelerator mass spectrometry with a gas-filled magnet. The measurements of 10Be, 14C, 39Ar, 59Ni -- and potentially of 131Xe -- can be performed in the same granitic sample that was already analyzed for 36Cl, 41Ca, 6Co, 152Eu, and 154Eu. This will provide extensive information on the neutron spectrum at the specified location, and similarly complete analyses can conceivably be performed on granite samples at other locations.

Neutron spectrum and yield of the Hiroshima A-bomb deduced from radionuclide measurements at one location.

In this paper measurements of the radionuclides of 36Cl, 41Ca, 60Co, 152Eu and 154Eu in samples from Hiroshima, which were exposed to neutrons of the A-bomb explosion, are interpreted. In order to calculate the neutron spectrum at the sample site, neutron transport calculations using Monte Carlo techniques were carried out. Activation profiles in a granite mock-up irradiated with reactor neutrons could be reproduced by this method using DS86 input parameters. The calculated neutron spectrum at the sample site for non-thermal neutrons is identical to that obtained in DS86, but contains some 50% more thermal neutrons. The influence of parameters like soil composition, source terms and air humidity on the activation of these radioisotopes is discussed. The granite-covered earth at the sample site, for example, hardens the spectrum in comparison with DS86 values. Even when using a fission spectrum pointing downward and neglecting air humidity one cannot explain our 36Cl measurements. If the effective thermal neutron fluences, that have a similar ratio of resonance integral to thermal neutron capture cross sections obtained from 36Cl, 41Ca and 152Eu, are averaged, a bomb yield of about 16 kt is deduced in agreement with a bomb yield of (15 +/- 3) kt estimated in DS86.

Accelerator mass spectrometry of 36Cl produced by neutrons from the Hiroshima bomb.

Accelerator mass spectrometry was performed at the Munich tandem laboratory to determine 36Cl/Cl ratios of samples from a tombstone exposed to neutrons from the Hiroshima bomb. The ratios were determined from the surface to deeper positions. The depth profile of 36Cl/Cl can be used for estimating the neutron energy distribution and intensity near the hypocentre in Hiroshima.