Charge distribution studies in the fast-neutron-induced fission of <Superscript>232</Superscript>Th, <Superscript>238</Superscript>U, <Superscript>240</Superscript>Pu and <Superscript>244</Superscript>Cm

Charge distribution studies for heavy-mass fission products were carried out in the fast-neutron-induced fission of ²³²Th, ²³⁸U, ²⁴⁰Pu and ²⁴⁴Cm using radiochemical and gamma-ray spectrometric techniques. The width parameter( σ_Z/σ_A), the most probable charge/mass ( Z _P/A _P), the charge polarization (ΔZ) and the slope of charge polarization [ δ(ΔZ)/δA ^′] as a function of the fragment mass (A ^′) were deduced. The average charge dispersion parameter ( 〈σ_Z〉) and proton odd-even effect ( δ_p) were also obtained for these fissioning systems. The 〈σ_Z〉 and δ_p values in the fissioning systems ²⁴¹Pu ^* and ²⁴⁵Cm ^* were determined for the first time. The δ(ΔZ)/δA ^′ value is also determined for the first time in the fissioning systems ²³⁹U ^* , ²⁴¹Pu ^* and ²⁴⁵Cm ^* . These data along with the literature data for even-Z fissioning systems such as ²³⁰Th ^* , ²³²Th ^* , ²³³U ^* , ²³⁴U ^* , ²³⁶U ^* , ²³⁸U ^* , ²³⁹Pu ^* , ²⁴⁰Pu*, ²⁴²Pu ^* , ²⁴⁶Cm ^* , ²⁵⁰Cf ^* and ²⁵²Cf(SF) are discussed in terms of nuclear structure effect and dynamics of descent from the saddle to the scission point. The role of the excitation energy in low-energy fission is also discussed. Received: 26 July 2002 / Accepted: 3 December 2002 / Published online: 3 April 2003 RID="a" ID="a"Present address: Emeritus Scientist (CSIR) Bhabha Atomic Research Centre, Nuclear Recycle Group, WIP Building, Trombay, Mumbai-400085, India; e-mail: rhiyer@magnum. barc.ernet.in Communicated by D. Schwalm     

Nuclear-charge polarization at scission in the 12 MeV proton-induced fission of <Superscript>232</Superscript>Th

The most probable charges of secondary fragments, produced after neutron evaporation from primary fragments, have been evaluated using fractional cumulative and mass yields in the 12MeV proton-induced fission of ²³²Th . The nuclear-charge polarization of primary fragments at scission has been obtained by correcting the most probable charge of secondary fragments for neutron evaporation. The fragment mass dependence of the nuclear-charge polarization at scission shows good agreement with that for thermal neutron-induced fission of ²³⁵U , indicating that the nuclear-charge polarization is nearly insensitive to mass and excitation energy of the fissioning nucleus for asymmetric fission in the actinide region.     

Evidence for a K<Superscript>π</Superscript> = 1/2<Superscript>+</Superscript> isomer in neutron-rich <Superscript>185</Superscript>Ta

In this paper we present for the first time the measured delayed neutron (DN) yields and time spectra from high-energy protons interacting with thick ^natPb targets. The 1GeV protons from the accelerator impinged on targets of different thicknesses producing a huge number of spallation-fission products, some of which can be DN precursors. After the beam is switched off, the DNs were detected with optimized ³He counter. The production yields of light DN precursors as ¹⁷N and “usual” fission products as ⁸⁷Br and ⁸⁸Br, which dominate the total DN activity, are obtained both for thin and thick targets. These new data are of great interest for the new generation high-power spallation targets based on liquid-metal technologies. Our findings also should help to constrain the physics models within the simulations codes.     

Neutron-neutron angular correlations in spontaneous fission of <Superscript>252</Superscript>Cf

An experiment has been carried out to study neutron-neutron angular correlations in spontaneous fission of ²⁵²Cf. Angular dependences of the number of neutron-neutron coincidences obtained in the experiment were compared with the results of the Monte Carlo calculations for various neutron detection thresholds in the range 425–1600 keV. It was inferred that 10–11% of the total number of prompt neutrons from ²⁵²Cf (s.f.) in the laboratory system were emitted isotropically and may probably be interpreted as neutrons directly associated with the instant of scission of the nucleus. The analysis allowed their energy distribution to be determined as well. A similar method was also used to describe the angular correlation of prompt neutrons that accompanied the reaction ²³⁵U(n _th ,f).     

Investigation of Ternary Fission of <Stack><Subscript>98</Subscript><Superscript>252</Superscript></Stack>Cf Using Three-Cluster and Unified Ternary Fission Models

Using three-cluster and unified ternary fission models, the ternary fission of ₉₈²⁵²Cf is studied. We applied collinear and equatorial configurations to study the ternary fission of ₉₈²⁵²Cf when the third fragment is ₃¹⁰Li. The nuclear potential energy in the three-cluster model and unified ternary fission model is calculated respectively, using Yukawa plus exponential and proximity formalisms. The relative yields of different fragmentation channels are calculated. Our results reveal that the ternary fragmentation potential of the three fragments and the relative yields depend on the configuration of three fragments and usedmodel. Two models predict that the lowest driving potential and highest relative yield take place for the fragment combination ₅₁¹³²Sb + ₄₄¹¹⁰Ru + ₃¹⁰Li. Also, the values of driving potential and relative yield are not equal in the three-clustermodel and unified ternary fission model. For fragment combination ₅₁¹³²Sb + ₄₄¹¹⁰Ru + ₃¹⁰Li, the relative yield based on the three-cluster model in collinear configuration is maximum, whereas the unified ternary fission model in equatorial configuration predicts the lowest relative yield.     

Ternary fission fragmentation of <Superscript>252</Superscript>Cf for all possible third fragments

The ternary fragmentation of ²⁵²Cf for all possible third fragments has been investigated using the recently proposed three-cluster model within a spherical approximation and satisfying the condition A ₁ 3 \geq A ₂ 3 \geq A ₃ . The most probable ternary configurations in the fission of ²⁵²Cf accompanied with all possible third fragment mass numbers from A ₃ = 1 to 84 are predicted and their independent and overall relative yields are calculated. The calculations of the properly charge minimized potential energy surface (PES) and yield reveal that even-mass third fragments are more favored than odd ones. In the most probable configuration having the minimum in the potential energy and the maximum in yield, among the three fragments, at least one (or two) of the fragment(s) associates itself with the neutron (or proton) closed shell and in some cases even with the doubly closed shell. The calculated relative yields imply that next to ¹⁴C (the heaviest third fragment observed in the spontaneous ternary fission of ²⁵²Cf , ^{34, 36, 38}Si , ^{46, 48}Ar , and ^{48, 50}Ca are presenting themselves as the most favoured cases to be observed as the third particle in the spontaneous ternary fission of ²⁵²Cf .     

Angular momenta of fission fragments in the α-accompanied fission of 252Cf

For the first time, average angular momenta of the ternary fission fragments ^{100, 102}Zr, ¹⁰⁶Mo, ^{144, 146}Ba and ^{138, 140, 142}Xe from the α-accompanied fission of ²⁵²Cf were obtained from relative intensities of prompt γ-ray transitions with the use of the statistical model calculation. Average values of the angular momenta were compared with the corresponding values for the same fission fragments from the binary fission of ²⁵²Cf. Results indicate the presence of a decreasing trend in the average values of angular momenta induced in ternary fission fragments compared to the same binary fission fragments. On the average, the total angular momentum extracted for ternary fission fragments is ∼1.4 ℏ lower than in binary fission. Consequently, results indicate that the mechanism of the ternary α-particles emission may directly effect an induction of angular momenta of fission fragments, and possible scenarios of such mechanisms are discussed. Further, the dependence of the angular momenta of ¹⁰⁶Mo and ¹⁴⁰Xe on the number of emitted neutrons from correlated pairs of primary fragments was obtained also showing a decreasing dependence of average angular momenta with increasing number of emitted neutrons. Consequences are briefly discussed.     

Collinear cluster tripartition as sequential binary fission in the <Superscript>235</Superscript>U(n<Subscript>th</Subscript>, f ) reaction

The mechanism leading to the formation of the observed products of the collinear cluster tripartition (CCT) is carried out within the framework of the model based on the dinuclear system concept. The yield of fission products is calculated using the statistical model based on the driving potentials for the fissionable system. The minima of potential energy of the decaying system correspond to the charge numbers of the products which are produced with large probabilities in the sequential fission (partial case of CCT) of the compound nucleus. The realization of this mechanism supposes the asymmetric fission channel as the first stage of sequential mechanism. It is shown that only the use of the driving potential calculated by the binding energies with the shell correction allows us to explain the yield of the true ternary fission products. The theoretical model is applied to research CCT in the reaction ²³⁵U(n _th, f). Calculations showed that the heavy products of two fission channels of ²³⁶U^*, ⁸²Ge^* + ¹⁵⁴Nd^* and ⁸⁶Se^* + ¹⁵⁰Ce^*, can undergo sequential fission forming the CCT products ⁷⁰Ni, ^{74, 76}Zn, ⁸⁰Ge and ⁸⁴Se with relatively large probabilities which can be observed in coincidence with corresponding partner nucleus. The obtained results can explain some of the observed CCT products Ni and Ge in coincidence with the Ge and Se isotopes in the experiments of the FOBOS group in Joint Institute for Nuclear Research.     

Cluster ion emission from LiF induced by MeV N<Superscript>q+</Superscript> projectiles and <Superscript>252</Superscript>Cf fission fragments

Ion cluster desorption yields from LiF were measured at PUC-Rio with ≈0.1 MeV/u N ^q+ (q = 2,4,5,6) ion beams by means of a time-of-fight (TOF) mass spectrometer. A ²⁵²Cf source mounted in the irradiation chamber allows immediate comparison of cluster emissions induced by ≈65 MeV fission fragments (FF). Emission of (LiF) _n Li⁺ clusters are observed for both the N beams and the ²⁵²Cf fission fragments. The observed cluster size n varies from 1 to 6 for N ^q+ projectiles and from 1 to ≈40 for the ²⁵²Cf-FF. The size dependence of the Y(n) distributions suggests two cluster formation regimes: (i) recombination process in the outgoing gas phase after impact and (ii) emission of pre-formed clusters from the periphery of the impact site. The corresponding distribution of ejected negative cluster ions (LiF) _n F⁻ closely resembles that of the positive secondary (LiF) _n Li⁺ ions. The desorption yields of positive ions scale as Y(n) ∼ q ⁵. A calculation with the CASP code shows that this corresponds to a cubic scaling ∼S _e ³ with the electronic stopping power S _e , as predicted by collective shock wave models for sputtering and models involving multiple excitons (Frenkel pair sputtering). We discuss possible interpretations of the functional dependence of the evolution of the cluster emission yield Y(n) with cluster size n, fitted by a number of statistical distributions.     

Production of neutron-rich nuclei in fission induced by neutrons generated by the p + <Superscript>13</Superscript>C reaction at 55 MeV

Cross-sections for the production of neutron-rich nuclei obtained by neutron-induced fission of natural uranium have been measured. The neutrons were generated by bombarding a ¹³C target with 55 MeV protons. The results, position of the maximum in the (Z, A)-plane, width and magnitude, are very comparable with those where the neutrons are generated by bombardment of natural ¹²C graphite with 50 MeV deuterons. Depending on the geometry of the converter/target assembly the isotope yields, however, are a factor of 2-3 lower due to less efficient production of neutrons per primary projectile, especially at small forward angles. Received: 8 November 2002 / Accepted: 20 December 2002 / Published online: 15 April 2003     

Spectra and mean energies of prompt neutrons from <Superscript>238</Superscript>U fission induced by primary neutrons of energy in the region <Emphasis Type="Italic">E</Emphasis><Subscript><Emphasis Type="Italic">n</Emphasis></Subscript><20 MeV

The time-of-flight technique is used to measure the ratios R(E, E _n )=N(E, E _n )/N_Cf(E) of the normalized (to unity) spectra N(E, E _n ) of neutrons accompanying the neutron-induced fission of ²³⁸U at primary-neutron energies of E _n =6.0 and 7.0 MeV to the spectrum N_Cf(E) neutrons from the spontaneous fission of ²⁵²Cf. These experimental data and the results of their analysis are discussed together with data that were previously obtained for the neutron-induced fission of ²³⁸U at the primary energies of E _n =2.9, 5.0, 13.2, 14.7, 16.0, and 17.7 MeV.     

Search for the emission of π<Superscript>0</Superscript> mesons from the neutron-induced fission of <Superscript>235</Superscript>U nuclei

A nuclear-reactor experiment on the search for the emission of neutral pions from the neutron-induced fission of ²³⁵U nuclei has been carried out. To this end, an experimental setup for searching for the emission of π⁰ mesons with high sensitivity to this process has been designed and produced. This setup consisted of two Cherenkov total-absorption spectrometers for the detection and measurements of the energy of two gamma-ray photons from π ⁰-meson decay. The spectrometers were placed at the exits of two coaxial horizontal experimental channels. To protect the detectors from low-energy β and γ rays and neutron fluxes, 3.5-m-long water filters were situated in the channels. To reject the cosmic background, large-area scintillation counters operating in the anticoincidence mode were placed over each spectrometer. The energy and time resolution of the spectrometers, as well as the efficiency of detecting charged particles by scintillation counters, were tested on the secondary electron beam of the Tomsk electron synchrotron Sirius. Runs of measurements of the effect on the operating reactor (duration of 805 h) were alternated with runs of measurements of background on the stopped reactor (duration of 403 h). Statistical processing of the experimental results yields an upper limit of ≤5.3×10 ^?12 with a 90% confidence level for the probability of the emission of neutral pions from the neutron-induced fission of ²³⁵U nuclei. This result and results of other works carried out with sources of spontaneously fissioning ²⁵²Cf nuclei show that the probabilities of the emission of π⁰ mesons from spontaneous fission and fission induced by fission-spectrum neutrons are equal to each other.     

Indication for hyperdeformed cluster states in <Superscript>233</Superscript>Th

An activation technique was used to investigate relative yields of fission products from the reaction ²³²Th(n, f ) for neutron energies between 1.3 and 1.8MeV covering the region around the first hyperdeformed resonances. Intensities of characteristic γ-ray transitions were analyzed to search for changes in the mass distribution for neutron energies corresponding to the resonances and below the resonances. Relative increases in yield between 7 and 23% are observed for A ≈ 100 and 132 in the resonance region around 1.6MeV. It is proposed that the yield enhancement of daughter nuclei of the preformed fragments ¹³²Sn and ¹⁰¹Zr arises from cold fission of a di-cluster configuration. The experimental results support theoretical predictions for the existence of hyperdeformed octupole shapes based on the di-nuclear configuration ¹³²Sn + ¹⁰¹Zr.     

Fission fragment γ-ray anisotropies

The anisotropy of fission fragment γ-rays in the reactions ²³⁹Pu(n_th, f) and ²³³U(n_th, f) have been measured. In this work, two γ energy bands were used to confirm the energy independence of the anisotropy. For the γ energy band of 0.49–0.65 MeV and the γ energy band of 0.83–0.92 MeV the anisotropies were found to be 0.18 ± 0.03, 0.13 ± 0.03 and 0.19 ± 0.03, 0.11 ± 0.03 for the ²³⁹Pu and ²³³U targets respectively. The data are corrected for the Doppler effect and the time of flight was large enough to eliminate the counting of neutrons. Comparisons with the theories of Nix and Swiatecki, and Strutinsky have been made and approximate correction for fragment rotation along fission axis made.     

Mass distribution studies in the <Superscript>19</Superscript>F + <Superscript>197</Superscript>Au reaction

Mass distribution and evaporation residue measurements have been carried out in the reaction ¹⁹F + ¹⁹⁷Au using the recoil catcher technique followed by off-line γ-ray spectrometry. The random neck rupture model (RNRM) has been used to compute the variance of the mass distribution ( σ²_A) and the average kinetic energy ( ˉ) of the fission fragments for the present system. The results of model calculations have been found to be in good agreement with the experimental observations. Measured evaporation residue cross-sections have been compared with the statistical model calculations.     

Mean energies of prompt fission neutrons in the neutron-induced fission of <Superscript>235</Superscript>U at primary energies in the range <Emphasis Type="Italic">E</Emphasis><Subscript>n</Subscript> < 20 MeV

The spectra of neutrons accompanying the induced fission of ²³⁵U target nuclei are described theoretically. It is confirmed that a third neutron source must be introduced in order to reproduce the shape of experimental distributions at high energies of primary neutrons (previously, a third source was used in describing the spectra of neutrons emitted in ²³²Th and ²³⁸U fission). On the basis of experimental results and their analysis, the mean energy of fission neutrons is estimated as a function of the bombarding-neutron energy up to E _n = 20 MeV.     

Prompt-fission-neutrons spectra of <Superscript>238</Superscript>U

The spectra of prompt fission neutrons from the reaction ²³⁸U(n, F) for neutrons of energy in the range E _n ≤ 20 MeV are interpreted within the statistical model. It is shown that exclusive spectra of prefission neutrons emitted in (n, xnf) reactions play a decisive role in describing the observed promptfission-neutron spectra and determine the average energies of prompt-fission neutrons. The dependence of the effect of prefission neutrons on the fissility of a target nucleus is demonstrated for the reactions ²³²Th(n, F), ²³⁵U(n, F), and ²³⁹Pu(n, F).     

Single-particle spin effect on fission fragment angular momentum

Independent isomeric yield ratios (IYR) of ¹²⁸Sb, ¹³⁰Sb, ¹³²Sb, ¹³¹Te, ¹³³Te, ¹³²I, ¹³⁴I, ¹³⁶I, ¹³⁵Xe, and ¹³⁸Cs have been determined in the fast neutron-induced fission of ²⁴³Am using the radiochemical and γ-ray spectrometric technique. From the IYR, fragment angular momenta (J _rms) have been deduced using the spin-dependent statistical model analysis. From the J _rms-values and experimental kinetic energy data deformation parameters (β) have been deduced using the pre-scission bending mode oscillation model and the statistical model. The J _rms- and β-values of fission fragments from the present and earlier work in the odd-Z fissioning systems ( ²³⁸Np ^* , ²⁴²Am ^* and ²⁴⁴Am ^* ) are compared with the literature data in the even-Z fissioning systems ( ^{230, 233}Th ^* , ^{233, 234, 236, 239}U ^* , ^{239, 240, 241, 242}Pu ^* , ²⁴⁴Cm(SF), ^{245, 246}Cm ^* , ²⁵⁰Cf ^* and ²⁵²Cf(SF)) to examine the role of single-particle (proton) spin effect. It was observed that i) in all the fissioning systems J _rms- and β-values of the fragments with spherical 82n shell and even-Z products are lower than the fragments away from the spherical neutron shell and odd-Z products, which indicate the effect of nuclear structure. ii) For both even-Z and odd-Z fission products J _rms-values increase with Z _F ²/A _F due to increase in Coulomb torque. iii) The J _rms- and β-values of even-Z fission products are comparable in all the fissioning systems. However, for odd-Z fission products they are slightly higher in the odd-Z fissioning systems compared to their adjacent even-Z fissioning systems. This is possible due to the contribution of the extra single-particle (proton) spin of the odd-Z fissioning systems to their odd-Z fragments. iv) The yield-weighted fragment angular momentum and elemental yields profile shows an anti-correlation in even-Z fissioning systems but not in the odd-Z fissioning systems.     

Study of α-particles produced in thermal neutron induced reactions on 235U

The ²³⁵U(n_th, α) reaction and the α-particles emitted in the thermal neutron induced fission of ²³⁵U were measured using a very pure thermal neutron beam of the Grenoble high flux reactor. An upper limit of 0.66 mb was determined for the ²³⁵U(n_th, α) reaction cross section, which is lower than all the previous results. The energy distribution of the α-particles produced by the ²³⁵U(n_th, f) reaction was measured down to 7 MeV with a non-shielded surface-barrier detector telescope assembly. The measured distribution has a quasi-Gaussian shape; it reveals, however, a pronounced deviation from such a shape at lower α-energies. Several possible explanations for this deviation are discussed.     

Gamma rays of primary fission products from 235U(n,f) and 239Pu(n,f)

Gamma rays of primary fission products in thermal-neutron-induced fission of ²³⁵U and ²³⁹Pu were investigated. Isotopic assignments of several lines were made by comparing fission yield ratios and relative γ-ray intensities of the two fissioning nuclei. Differences between ²³⁵U and ²⁵²Cf fission product γ-ray lines are discussed.