Study of many-nucleon correlations in32S as a model for fragment shell effects in fission

The formation and break-up of substructures is studied in³²S as a calculable microscopic model for analogous long-range many-nucleon correlations in the fission of actinides. The calculations are performed for alpha-cluster wave functions with Volkov and Brink-Boeker interaction allowing forα,¹²C,¹⁶O and²⁰Ne clustering. It turns out that the correlated motion of large magic numbers of nucleons in two groups (¹⁶O+¹⁶O) is energetically favorable already at relatively small deformations. In the second minimum the¹⁶O+¹⁶O substructure occurs with high probability (about 80%). In analogy to these results the “pre-formation” of fragments and “fragment shell” effects occuring in the fission of actinides are explained in terms of probability statements for the formation of the corresponding heavy clusters in the many-body wave function.     

Photonuclear reactions of actinides in the giant dipole resonance region

Photonuclear reactions at energies covering the giant dipole resonance (GDR) region are analyzed with an approach based on nuclear photoabsorption followed by the process of competition between light-particle evaporation and fission for the excited nucleus. The photoabsorption cross-section at energies covering the GDR region is contributed by both the Lorentz-type GDR cross-section and the quasi-deuteron cross-section. The evaporation-fission process of the compound nucleus is simulated in a Monte Carlo framework. Photofission reaction cross-sections are analyzed in a systematic manner in the energy range of ∼ 10-20 MeV for the actinides ²³²Th , ²³⁸U and ²³⁷Np . Photonuclear cross-sections for the medium-mass nuclei ⁶³Cu and ⁶⁴Zn , for which there are no fission events, are also presented. The study reproduces satisfactorily the available experimental data of photofission cross-sections at GDR energy region and the increasing trend of nuclear fissility with the fissility parameter Z ²/A for the actinides.     

Symmetric and asymmetric fission modes in proton-induced fission at 660 MeV of <Superscript>238</Superscript>U

Fission product cross sections of intermediate-energy fission of ²³⁸U were used in order to construct the charge and mass yield distributions. Enriched target of ²³⁸U was irradiated by proton beam with energy 660 MeV for several hours at the LNP Phasotron, Joint Institute for Nuclear Research (JINR), Dubna, Russia. The charge distribution of the fission fragments was analyzed for calculation of isobaric cross sections. The mass yield curves were expanded into symmetric and asymmetric components according multimodal fission approach. The fissility values of actinides were calculated at given proton energy. The obtained results have been compared to the same data for targets ²³⁷Np and ²⁴¹Am.     

Investigations of fission characteristics and correlation effects

We review the experimental results on the P-even and P-odd angular correlations of fission fragments in the fission of the ²³⁵U and ²³⁹Pu nuclei induced by unpolarized and polarized resonance neutrons, and on the TRI and ROT effects in the ternary and binary fission of actinides induced by polarized thermal neutrons. Also reported are the measured yields of prompt and delayed neutrons per fission event. The experimental data are analyzed within a novel theoretical framework developed by the JINR—RNC KI Collaboration, whereby the reduction of the multidimensional phase space of fission fragments to the JπK-channel space is consistently validated and the role of resonance interference in the observed correlation effects is revealed.     

Fission experiments with secondary beams

Nuclear fission from excitation energies around 11 MeV was studied at GSI, Darmstadt for 76 neutron-deficient actinides and pre-actinides by use of relativistic secondary beams. The characteristics of multimodal fission of nuclei around ²²⁶Th are systematically investigated and related to the influence of shell effects on the potential-energy and on the level density between saddle point and scission. A systematic view on the large number of elemental yields measured gave rise to a new interpretation of the enhanced production of even elements in nuclear fission and allowed for a new understanding of pair breaking in fission.     

Spontaneous fission in actinides and heavy elements: A semiclassical view

The systematics of spontaneous fission in actinides and heavy elements are investigated within the framework of the semiclassical quantization. The interaction barrier is calculated by using the asymmetric two-centre shell model and its appropriate parameterization generates the analytical expression for the tunneling probability. The powerful semiclassical quantization technique lifts the degeneracy between the degenerate levels just after tunneling across the barrier. Our results clearly show that dissipation enhances the tunneling rate. It has also been seen that the sub-barrier fission from the excited state is a slow process. An appropriate condition for the fission isomeric state is also pointed out. The survival probability of heavy elements is a remarkable outcome of our model. We have tested our model for nuclei ₉₂ ²³⁶U , ₉₈ ²⁵²Cf , ₁₀₀ ²⁵⁴Fm and ₁₀₂ ²⁵²No .     

Measurements of delayed-neutron yields from thermal-neutron-induced fission of 235U, 233U, 239Pu, and 237Np

The experimental results on delayed-neutron yields from thermal-neutron-induced fission of some actinides in the IBR-2 pulsed reactor are presented. A method of periodic irradiation without displacement of the sample was used. The measurements of delayed-neutron total yields in thermal-neutron-induced fission of ²³⁹Pu, ²³³U, and ²³⁷Np and in cold-neutron-induced fission of ²³⁵U, ²³³U, and ²³⁹Pu were carried out. All values were obtained with the use of the value of β₀ for (n _th+²³⁵U) as a reference. Precise measurements of decay curves in the time interval 5–350 ms for ²³⁵U and ²³⁹Pu were performed.     

Intranuclear-Cascade model calculation of photofission probabilities for actinide nuclei

We have calculated the fission probabilities for ²³⁷Np, ^{233, 235, 238}U, ²³²Th, and ^natPb following the absorption of photons with energies from 68 MeV to 3.77 GeV using the RELDIS Monte Carlo code. This code implements the cascade-evaporation-fission model of intermediate-energy photonuclear reactions. It includes multiparticle production in photoreactions on intranuclear nucleons, pre-equilibrium emission, and the statistical decay of excited residual nuclei via competition of evaporation, fission, and multifragmentation processes. The calculations show that in the GeV energy region the fission process is not solely responsible for the entire total photoabsorption cross-section, even for the actinides. The fission probabilities are 80-95% for ²³³U, ²³⁵U, and ²³⁷Np, 70-80% for ²³⁸U, and only 55-70% for ²³²Th. This is because certain residual nuclei that are created by deep photospallation at GeV photon energies have relatively low fission probabilities. The results of those model calculations are in reasonable agreement (at the 10% level) with recent experimental data on relative photofission cross-sections for ²³⁷Np and ^{233, 235, 238}U (but not for ²³²Th or ^natPb) from the Saskatchewan and Jefferson Laboratories over a very wide range in photon energy. Using our calculated fission probabilities plus the total photoabsorption cross-sections per nucleon, estimated from previous cross-section data for nuclei from C to Pb, we can infer absolute photofission cross-sections for the actinide nuclei and compare them with the SAL and JLab results. The resulting discrepancies, however, clearly demonstrate the need for direct measurement of the total photoabsorption cross-sections for the heavy actinides.     

Determination of neutron-induced fission cross-sections of unstable nuclei via surrogate reaction method

Heavy ion reaction studies around Coulomb barrier energies have been generally used to investigate the effect of the structure of projectile/target on reaction dynamics. Other than providing an understanding of basic physics of the reaction dynamics, some of these reactions have been used as tools to serve as surrogates of neutron-induced compound nuclear fission cross-sections involving unstable targets. In this paper, we report some of the recent results on the determination of neutron-induced fission cross-sections of unstable actinides present in Th–U and U–Pu fuel cycles by surrogate reaction method by employing transfer-induced fission studies with ^6,7Li beams.     

Results of the searches for superheavy nuclei in the Cheleken Penninsula geothermal waters

The water rich in heavy volatile metals form the Cheleken Penninsula hot springs was passed through a column containing 850 kg of anion exchange resin. The spontaneous fission activity (SF) of the samples was measured by neutron multiplicity detectors. The counting rate of spontaneous fission events was 0.5 per day for 9 kg of saturated resin. After 170 kg of the resin had been treated with acid solutions and hydroxides had been precipitated from the eluate with alkali, the counting rate for the precipitate was about five per day. From measurements of theα/SF ratio it is concluded that the activity cannot be traced back to a contamination by actinides, except to a contamination by pure²⁵²Cf, which, however, seems to be unlikely. Thus the explanation of the observed effect as being due to the spontaneous fission of a new naturally occurring isotope of a superheavy element is considered to be the most probable one.     

A general framework for describing photofission observables of actinides at an average excitation energy below 30 MeV

A reasonable prediction of photofission observables plays a paramount role in understanding the photofission process and guiding various photofission-induced applications, such as short-lived isotope production, nuclear waste disposal, and nuclear safeguards. However, the available experimental data for photofission observables are limited, and the existing models and programs have mainly been developed for neutron-induced fission processes. In this study, a general framework is proposed for characterizing the photofission observables of actinides, including the mass yield distributions (MYD) and isobaric charge distributions (ICD) of fission fragments and the multiplicity and energy distributions of prompt neutrons (n_p) and prompt γ rays (γ_p). The framework encompasses various systematic neutron models and empirical models considering the Bohr hypothesis and does not rely on the experimental data as input. These models are then validated individually against experimental data at an average excitation energy below 30 MeV, which shows the reliability and robustness of the general framework. Finally, we employ this framework to predict the characteristics of photofission fragments and the emissions of prompt particles for typical actinides including ²³²Th, ^{235, 238}U and ²⁴⁰Pu. It is found that the ²³⁸U(γ, f) reaction is more suitable for producing neutron-rich nuclei compared to the ²³²Th(γ, f) reaction. In addition, the average multiplicity number of both n_p and γ_p increases with the average excitation energy.     

On the quest of production of superheavy nuclei in reactions of 48Ca with the heaviest cctinide targets

The sequence of radioactive decays of an unknown isotope produced in a rare fusion reaction to known lighter isotopes is used to identify mass and atomic number of the mother isotope, which has been separated before from the bulk of other reaction products by an in-flight recoil separator. By this technique the elements 107 to 112 were produced by single atom decay-chain analysis. Such a correlation technique reaches its limit by the occurrence of accidental sequences and it collapses beyond a maximum possible correlation time, at which a true event cannot be distinguished anymore from a random event. ⁴⁸Ca-induced fusion reactions with actinides are discussed. In 1983 at GSI, Darmstadt and LBL, Berkeley, ⁴⁸Ca/²⁴⁸Cm-experiments (II) were performed, which are compared to recent ⁴⁸Ca-experiments at FLNR-Dubna (I) irradiating ²⁴⁴Pu, ²⁴²Pu, and ²³⁸U. In these experiments production of isotopes of superheavy elements 112 and 114 is claimed. Our analysis of accidental sequences in ⁴⁸Ca-induced reactions is presented, which is at variance with the published analysis from FLNR-Dubna. We find that the maximum correlation time using continuous beams at today existing separation systems is not in the one-hour regime, but in the few-minute regime. The five spontaneous fission events observed in the FLNR experiments are preceded by signals in the (1–16)-minute range. These times are shown to be longer than the maximum possible correlation times. The preceding signals are decoupled from the spontaneous fission signal and carry no information on the spontaneous fission events observed. Moreover, random probabilities of 0.2 to 0.6 for the signals preceding the fission events indicate that the correlations are of random origin. The evidence to have discovered element 114 in the reported experiments is classified “very weak”. Received: 13 October 1999     

Energetics of the fission process

The mass asymmetry of fragments from nuclear fission of heavy nuclei is reviewed. While mass asymmetry is a common and well-known phenomenon for low-energy fission of the lighter actinides, more recent experiments have demonstrated that, for the heaviest actinides, the mass distribution switches to a symmetric one. On the other hand, it has been discovered that, though for fissioning nuclei with mass numbersA225 the mass distribution is basically symmetric, an asymmetric component is clearly to be identified for nuclei down to the Pb-region. In the absence of a generally accepted dynamical theory of fission, the above experimental findings are discussed in terms of static energy considerations. Triggered from the outset by the structure of the potential energy surface at the saddlepoint, the energy balance at the scission point between the available energy (Q-value) of the reaction and the Coulomb and deformation energy of the nascent fragments is shown to steer the characteristics of the fragment mass distributions.     

Application of pulse shape discrimination in Si detector for fission fragment angular distribution measurements

Pulse shape discrimination (PSD) with totally depleted transmission type Si surface barrier detector in reverse mount has been investigated to identify fission fragments in the presence of elastic background in heavy ion-induced fission reactions by both numerical simulation and experimental studies. The PSD method is compared with the other conventional methods adopted to identify fission fragments with solid-state detectors such as ΔE–E telescope and single thin ΔE detector and the data for the¹⁰B +²³²Th fission reaction are presented. Results demonstrate the usefulness of a single transmission-type surface barrier detector for the identification of fission fragments and projectiles like heavy ions     

Heavy element nuclear chemistry at JAERI

The present status of heavy element nuclear chemistry research at JAERI (Japan Atomic Energy Research Institute) is reviewed. Production of the transactinide nuclei ²⁶¹Rf and ²⁶²Db via the reactions of ²⁴⁸Cm(¹⁸O,5n) and ²⁴⁸Cm(¹⁹F, 5n), respectively, at the JAERI tandem accelerator is reported. Study of the aqueous chemistry of Rf is being carried out with a newly developed rapid ion-exchange separation apparatus. Anion-exchange behavior of Rf in acidic solution is briefly discussed. Recent experimental results on decay studies of neutron-deficient actinide nuclei using the gas-jet coupled JAERI-ISOL are given. We also discuss characteristics of nuclear deformation properties at scission in symmetric and asymmetric fission of actinides. Prospects for studies in the near future are briefly considered.     

Odd-even effect in fragment angular momentum in low-energy fission of actinides

Quantitative explanation for the odd-even effect on fragment angular momenta in the low-energy fission of actinides have been provided by taking into account the single particle spin of the odd proton at the fragment’s scission point deformation in the case of odd-Z fragments along with the contribution from the population of angular momentum bearing collective vibrations of the fissioning nucleus at scission point. The calculated fragment angular momenta have been found to be in very good agreement with the experimental data for fragments in the mass number region of 130–140. The odd-even effect observed in the fragment angular momenta in the low-energy fission of actinides has been explained quantitatively for the first time.      

The isotopes259106,260106, and261106

In irradiations of²⁰⁷Pb and²⁰⁸Pb, respectively, with⁵⁴Cr theα-decay of the isotopes²⁵⁹106,²⁶⁰106, and²⁶¹106 could be observed for the first time. For²⁶⁰106 a spontaneous fission branch of (50 _?20 ⁺³⁰ )% was observed. The isotopes were identified by genetic relationships of α-decay after separation in-flight with the velocity filter SHIP and implantation into a position-sensitive silicon surface-barrier detector. The measured partial fission halflife of the doubly even isotope²⁶⁰106 of (7.2 _?2.7 ^+4.8 )ms exceeds the predicted values by at least a factor of 40. This result could be explained by the high shell corrections of the ground state mass, derived from the measured α-decay energies. The experimental results show evidence for an island of purely shell stabilized nuclei in the region of deformed isotopes beyond the actinides.     

Innovative separation method for advanced spent fuel reprocessing based on tertiary pyridine resin

Radiochemical separation experiments have been performed in order to realize a novel reprocessing method based on chromatography techniques using a novel pyridine resin. The newly synthesized tertiary pyridine resin with two functions of ion exchanger and soft-donor was dedicated to the experiments, where highly irradiated mixed oxide fuel from the experimental fast reactor JOYO was used as a reference spent fuel. With a 3-step separation, pure Am and Cm were individually obtained as minor actinide products, and ¹⁰⁶Ru group, lanthanides with ¹³⁷Cs group and Pu group were fractionated, respectively. The decontamination factor of ¹³⁷Cs and trivalent lanthanides (¹⁵⁵Eu, ¹⁴⁴Ce) against the Am product exceeded 3.9 × 10⁴ and 1.0 × 10⁵, respectively. The decontamination factor as the mutual separation of ²⁴³Cm was larger than 2.2 × 10³ against the Am product. Moreover, the content of ¹³⁷Cs, trivalent lanthanides and ²⁴³Cm in Am product did not exceed 2 ppm. The tertiary pyridine resin method is a candidate separation system for an “advanced ORIENT process”, where enhanced separation, transmutation and utilization of actinides, long-lived fission products and rare metal fission product would be oriented.     

New conditionings for separated long-lived radionuclides

Long-lived radionuclides such as I¹²⁹, Cs¹³⁵ and minor actinides can be incorporated in crystalline structures of several specific materials with high chemical durability. Apatites, zirconolite, monazites, thorium phosphate-diphosphate and hollandite are being studied at the CEA and among a scientific research group called NOMADE. A first step is devoted to the scientific feasibility dealing with elaboration and characterization of non-radioactive materials and studies of their chemical durability and radiation stability. Development of apatite for iodine and minor actinides, zirconolite for minor actinides, monazite for trivalent actinides and thorium phosphate–diphosphate for tetravalent actinides has reached the scientific feasibility. Cs conditioning in hollandite and phosphate minerals needs further studies. To cite this article: C. Guy et al., C. R. Physique 3 (2002) 827–837.     

Nuclear cluster structure: Superheavies, cluster-radioactivity and exotic fission processes

The extension of the periodic system into various new areas is investigated. Experiments for the synthesis of superheavy elements and the predictions of magic numbers are reviewed. Different channels of nuclear decay are discussed like cluster radioactivity, cold fission and cold multifragmentation, including the recent discovery of the tripple fission of ²⁵²Cf.