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     

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.     

Systematics of charge distribution studies in low-energy fission of actinides

Charge distribution studies were carried out in the thermal neutron-induced fission of ²²⁹Th, ²⁴¹Pu and ²⁴⁵Cm as well as in the spontaneous fission of ²⁵²Cf. The width parameter (σ_z/σ_A), the most probable charge/mass (Z_p/A_p) and the charge polarization (ΔZ) as a function of fragment mass were deduced. The slope of charge polarization as a function of fragment mass [δ(ΔZ)/δA′], average charge dispersion parameter (〈σ_z〉) and proton odd-even effect (δ_p) were also obtained for these fissioning systems. These data along with the literature data for even-Z fissioning systems such as ²³³Th¹, ²³³U¹, ²³⁴U¹, ²³⁶U¹, ²³⁹U¹, ²³⁹Pu¹, ²⁴⁰Pu¹ and ²⁵⁰Cf¹ are discussed in terms of nuclear-structure effects and dynamics of descent from saddle point to the point of neck formation and from the formation of the neck to the scission point.     

Fission yields at different fission-product kinetic energies for thermal-neutron-induced fission of 239Pu

At the recoil spectrometer “Lohengrin” of the Institut Laue-Langevin in Grenoble, the yields of the light fission products from the thermal-neutron-induced fission of ²³⁹Pu were measured as a function of A, Z, the kinetic energy E and the ionic charge states q. The nuclear charge and mass distributions summed over all ionic charge states were determined for different light fissionproduct kinetic energies between 93 and 112 MeV. The proton odd-even effect which was measured to be (11.6 ± 0.6)% causes considerable fine structure in the yields. The average kinetic energy of even-Z elements in the light fission-product group is 0.3 ± 0.1 MeV larger than for odd-Z elements. The neutron odd-even effect is (6.5 ± 0.7)%. The comparison with previously published data ¹) for thermal-neutron-induced fission of ²³⁵U reveals a correlation between the proton odd-even effect in the yield and in the kinetic energy of the elements. The dependence of the proton odd-even effect on the fragmentation is very similar for ²³⁵U and ²³⁹Pu when it is considered as a function of the nuclear charge of the heavy fission products. The isobaric variances σ_z². for thermal-neutron fission of ²³⁵U and ²³⁹Pu coincide at all kinetic energies if the influence of the proton odd-even effect is averaged out. This supports the hypothesis that the magnitude of σ_z² is determined only by quantum-mechanical zero-point fluctuations. The influence of the spherical shells Z = 50 and N = 82 on the fragmentation is discussed.     

Nuclear charge distribution of mass-separated isobars from thermal-neutron-induced fission of 235U

The nuclear charge distribution of fission products with mass numbers A = 90, 91, 94, 99, 100, 101 and 104 provided by the mass separator “Lohengrin” was measured. Adjacent elements in the group of the light fission products could be separated by their different energy loss in a carbon absorber. The Z-yields were found to be strongly dependent on the kinetic energy of the fission products. The widths of the nuclear charge distributions are very small, in general, and strongly dependent on A as well as on the kinetic energy. The influence of the neutron evaporation and odd-even effects are clearly detected. An asymmetric nuclear charge distribution was found for A = 104 indicating the suppression of fission fragments with Z = 43. The average nuclear charges of the fission products at their average kinetic energy are in good agreement with the results from measurements of the number of β-decays and K X-ray measurements. The average nuclear charge of the isobar A = 132 was measured at its average kinetic energy with a calibrated secondary electron detector to be Z = 51.14 ± 0.15 which is in very good agreement with the radiochemical results. Thus previous physical measurements indicating a large independent yield for the doubly magic nucleus ¹³²Sn could not be confirmed.     

The influence of pairing and nuclear structure on the thermal-neutron-induced fission of235U

The mass separated fission product beam provided by the mass separator “Lohengrin” has been used to determine the nuclear charge distribution for the thermal-neutron-induced fission of²³⁵U for all light fission products in the region 80≦A≦107. The measurements were performed at the most probable kinetic energy of the fission products. By using the known fission product mass yields, the independent yields for a total number of 100 nuclides were obtained under the condition of the most probable kinetic energy. The proton pairing effect modulates the average nuclear charge of the fission fragments and the isobaric charge distribution widths in a regular fashion. The probabilities of breaking a pair and of forming fragments with an energetically unfavourable neutron-to-proton ratio are found to compete with each other. Both probabilities depend on the mass split and reach their maximum values in the region of the most probable masses. The odd-even-proton effect is found to vary smoothly between 16% for the most abundant mass splits and 40% for the rare mass splits. The odd-even-neutron effect exhibits maxima nearN=50 andN=60, where it reaches 16%. These maxima and the extremely low Tcyield (0.13±0.05%) are discussed with regard to fragment shell effects.     

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.     

Mass distribution in the bremsstrahlung-induced fission of Th,U and Pu

The yields of various fission products in the 10 MeV bremsstrahlung-induced fission of ²³²Th, ²³⁸U and ²⁴⁰Pu were determined using a recoil catcher and off-line γ-ray spectrometric techniques. From the yield data, mass yield distributions were obtained using charge distribution corrections. The higher yields of fission products around mass numbers 133–135, 138–140, 143–145 and their complementary products in the neutron and bremsstrahlung-induced fission of ²³²Th, ²³⁸U and ²⁴⁰Pu were interpreted based on nuclear structure effects. From the mass yield distribution, the peak-to-valley (P/V$P/V$) ratio was also obtained for the above fissioning systems. The present data, along with data from the literature on different bremsstrahlung- and mono-energetic neutron-induced fissions of ²³²Th and ²³⁸U are interpreted to examine the influence of excitation energy on the peak to valley ratio. For the same compound nucleus ²⁴⁰Pu^?, the data in the 10–30 MeV bremsstrahlung-induced fission of ²⁴⁰Pu were compared with similar data of thermal to 14 MeV neutron-induced fission of ²³⁹Pu and the spontaneous fission of ²⁴⁰Pu to examine the role of excitation energy due to bremsstrahlung radiation and mono-energetic neutrons.     

Systematics of asymmetry in fission based on order-disorder model

According to Order-Disorder Model (ODM), in the early stages of fission, the charges in a fissioning nucleus gets polarised into two impending parts along with corresponding most stable neutrons which are calculated from the minimum in isobaric mass parabola. This polarisation into two most stable configuration leaves a small number of neutrons as balance neutrons i.e.N _bal. The distribution of theseN _bal for various polarisation modes, shows a very profound correlation with the yield distribution. Judging from this striking correlation between these two distributions, it can be predicted that the asymmetry in fission decreases gradually and ultimately disappear for nuclei havingZ ⋍ 102 but reappears again for the nuclei in super heavy region.     

Fragment angular momenta in low and medium energy fission of242Pu

Independent isomeric yield ratios of¹²⁸Sb were determined radiochemically in the thermal neutron induced fission of²⁴¹Pu and 34 MeV alpha particle induced fission of²³⁸U, both involving the same compound nucleus (²⁴²Pu). Fragment angular momenta estimated from the measured isomer ratios using the statistical model analysis showed significantly larger fragment angular momenta in the medium energy fissioning system compared to the low energy fissioning system. This has been attributed to the effect of higher excitation energy and angular momentum in the entrance channel leading to increased fragment temperature, moments of inertia and angular velocity. An attempt was made to calculate the fragment angular momentum in the medium energy fission using the Fermi gas model for the fissioning nucleus, taking into account the multichance fission, saddle shapes of the fissioning nuclei and the angular velocity components of the fissioning nuclei both along and orthogonal to the fission axis. The calculated angular momenta agree well with the experimental results.     

Fragment mass dependence of angular anisotropy in 15 MeV proton-induced fission of 244Pu

Angular distributions of fission fragments with mass number A=97-159 have been measured by the radiochemical recoil-catcher method in the proton-induced fission of ²⁴⁴Pu with the incident energy of 15 MeV. Angular anisotropies of extreme asymmetric mass division products even up to the fragment mass ratio of A _H /A _L ∼ 1.85 are found not any different from those of the typical asymmetric mass division products with A∼ 138, which indicates that no clear evidence is observed for the existence of an additional saddle point configuration in the extreme asymmetric mass division. The correlation between the saddle point state evaluated from the angular anisotropy and the mass division mode is discussed.     

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.     

Nuclear-charge polarization at scission in proton-induced fission of <Superscript>233</Superscript>U

The primary and the secondary fragment mass yields and neutron multiplicity in the 11.5MeV proton-induced fission of ²³³U were determined by a double time-of-flight method. The most probable charges of the secondary fragments in the isobaric chains with A = 126 , 127, 129, 132, and 136 have been derived from the secondary mass yields together with the literature values of the fractional cumulative and independent yields measured radiochemically. The nuclear-charge polarization of primary fragments at scission was obtained by correcting the secondary fragment mass for neutron evaporation. The results show that the nuclear-charge polarization is mostly determined by the minimum potential energy of nuclei at scission and that this behavior is nearly independent not only of mass and excitation energy but also of neutron-to-proton ratios of the fissioning nuclei.     

Studies of mass and energy correlations in thermal neutron fission of U-235 accompanied by long range alpha particles

Several characteristics of fission accompanied by long range alpha particles (LRA) have been studied in the thermal neutron induced fission of²³⁵U. The kinetic energies of fission fragments and the LRA were measured with a back-to-back ionization chamber and semiconductor detectors respectively. The kinetic energies of the two fragments and the LRA in LRA fission, along with the energies of pair fragments in the normal binary fissions, were recorded event by event on a magnetic tape by means of a four-parameter data acquisition system. The data were analysed to study the dependence of different quantities in LRA fission on the fragment mass ratio, LRA energy and the total kinetic energy of the fission fragments. It is seen that the most probable energy of LRA increases significantly for near symmetric mass divisions. The total kinetic energy for all mass ratios in LRA fission is found to be (2.6±0.7) MeV larger than that in binary fission. The difference in the total kinetic energies in LRA and binary fissions is seen to be dependent on mass ratio. This result may suggest that the scission configuration in LRA fission is different for different mass ratios. Correlations between the fission fragment and LRA energies have been studied for several mass ratios. It is seen that the most probable fragment kinetic energyĒ _k varies nearly linearly with the LRA energyE _a for various mass divisions but the variation of the most probable LRA energyĒ _a with fragment kinetic energyE _k is found to deviate from linearity for several mass ratios. From a least square fit to the variation ofĒ _k withE _a it is found that the slope (dĒ _k/dE_a) increases with the increase in mass ratio. The present results are discussed to arrive at a better understanding of the scission configuration in the fission accompanied by LRA emission.     

Indpeendent Yields of Iodine and Tellurium Isotopes in Fission of 232 Thorium with 30.5 MeV Alpha Particles

Iodine and tellurium isotopes produced in the fission of ²³²Th with 30.5 MeV alpha particles were separated using a method of sublimation in an air stream and the independent yields of ¹³⁰I, ¹³¹I, ^132m,gI, ¹³³I ¹³⁴I, ^134m,gTe, ^133mTe and ¹³⁴Te (cumulative) were determined by means of high resolution Ge(Li) γ-ray spectrometry. A Gaussian fit to the experimental data was used to obtain the width parameter σ_z and the most probable charge Z_p of the nuclear charge distribution in the isobaric chains 130 – 131. The most probable masses for fission fragments with Z = 52 and Z = 53 were also deduced from the measured fission yields.     

Fission-fragment energy correlation measurements for the spontaneous fission of 244Cm

Fission-fragment mass and kinetic energy distributions and their correlations have been measured for the spontaneous fission of ²⁴⁴Cm. About 3.54 × 10⁵ fission events were collected. The global mass distribution shows shoulders at μ_H ≈ 134 and μ_H ≈ 143?144. The peak/valley ratio is 86. The dip ΔE_K value at symmetry is 13.4 ± 1.5 MeV. In the yields for high-kinetic-energy selected events, the masses 139 and 144 dominate. The results of ²⁴⁴Cm are compared with the other isotopes of Cm and discussed in terms of the structures present in the potential energy surface of the fissioning system caused by the structures in the nascent fragments.     

Long-range alpha emission inP-wave neutron induced fission of235U

The yield and energy distribution of long-range alpha-particles (lra) emitted from neutron-induced fission of²³⁵U have been measured at neutron energies; thermal, 125±12, 155±11, 185±10, 210±9, 240±9, 365±50 and 480±45 keV. The long-range alpha-particles were detected in cellulose nitrate track detector foils. Results showed an increase of about 50% in the yield at neutron energies in the region 150 keV≤E _n≤220 keV as compared to that of thermal neutrons. A calculation has been carried out to extract thelra to binary fission ratio forp-wave neutron induced fission.     

Distinction between pre-formed cluster emission and heavy ion decay by fission

For studying cluster radioactivity in the actinide region as well as trans-tin region two types of models are used: the pre-cluster formation model and the unified fission model. In the case of the actinide region, the cluster-like shapes are preferred for very high asymmetry while fissioning shapes are more suitable for less asymmetry and symmetry (the line of demarcation being around A _c =31). In this work this line of demarcation is studied in the case of the trans-tin region. The results of this study show that the transition from cluster mode to fission mode takes place at A _c =16.     

Fission fragment angular distribution in alpha-particle-induced fission of actinide elements

Using Lexan polycarbonate plastic as the fission fragment track detectors, the fragment angular distributions have been measured in the cases of fission of²³²Th and²³⁸U induced by alpha particles of various energies ranging from 40 to 70MeV obtained from the 88″ variable energy cyclotron at Calcutta. The center-of-mass angular distributions have been calculated and fitted by a series of Legendre polynomials. TheW(10°)/W(90°) ratios (defined as anisotropy) were measured at several energies for both the targets. These data are utilized in calculation of the energy dependence ofK ₀ ² , the standard deviation of the distribution in the angular momentum projection on the nuclear symmetry axis at the saddle point. Values of Γ _f /Γ _η , i.e. the ratio of the fission width to neutron emission width have been determined for²³²Th and²³⁸U nuclei. The integral cross-section for alpha induced fission in each target was determined by numerical integration of the respective center-of-mass angular differential cross-sections. The results were compared with similar data available in the literature which served to resolve some of the discrepancies observed in earlier measurements. The results were also compared with theoretical cross-sections.