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Binding energies of high-L Rydberg levels of Th{sup 3+} were measured using the resonant excitation Stark ionization spectroscopy technique. Analysis of the data with the long-range polarization model leads to determination of dipole and quadrupole polarizabilities of the free Th{sup 4+} ion, {alpha}{sub d} = 7.61(6) a.u., {alpha}{sub Q} = 47(11) a.u.
We have measured the reaction rates of trapped, buffer gas cooled Th{sup 3+} and various gases and have analyzed the reaction products using trapped ion mass spectrometry techniques. Ion trap lifetimes are usually limited by reactions with background molecules, and the high electron affinity of multiply charged ions such as Th{sup 3+} make them more prone to loss. Our results show that reactions of Th{sup 3+} with carbon dioxide, methane, and oxygen all occur near the classical Langevin rate, while reaction rates with argon, hydrogen, and nitrogen are orders of magnitude lower. Reactions of Th{sup 3+} with oxygen and methane proceed primarily via charge exchange, while simultaneous charge exchange and chemical reaction occurs between Th{sup 3+} and carbon dioxide. Loss rates of Th{sup 3+} in helium are consistent with reaction with impurities in the gas. Reaction rates of Th{sup 3+} with nitrogen and argon depend on the internal electronic configuration of the Th{sup 3+}.
Binding energies of high-L Rydberg states (L{>=} 7) of Th{sup 2+} with n = 27-29 were studied using the resonant excitation Stark ionization spectroscopy (RESIS) method. The core of the Th{sup 2+} Rydberg ion is the Fr-like ion Th{sup 3+} whose ground state is a 5 {sup 2}F{sub 5/2} level. The large-core angular momentum results in a complex Rydberg fine-structure pattern consisting of six levels for each value of L that is only partially resolved in the RESIS excitation spectrum. The pattern is further complicated, especially for the relatively-low-L levels, by strong nonadiabatic effects due to the low-lying 6d levels. Analysis of the observed RESIS spectra leads to determination of five properties of the Th{sup 3+} ion: its electric quadrupole moment Q = 0.54(4); its adiabatic scalar and tensor dipole polarizabilities {alpha}{sub d,0} = 15.42(17) and {alpha}{sub d,2} = -3.6(1.3); and the dipole matrix elements connecting the ground 5 {sup 2}F{sub 5/2} level to the low-lying 6 {sup 2}D{sub 3/2} and 6 {sup 2}D{sub 5/2} levels, |<5 {sup 2}F{sub 5/2}||D||6{sup 2}D{sub 3/2}>|=1.435(10) and |<5{sup 2}F{sub 5/2}||D||6{sup 2}D{sub 5/2}>|=0.414(24). All are in atomic units. These are compared with theoretical calculations.
High-resolution studies of the fine-structure pattern in high-L n = 37 levels of Th{sup 3+} have been carried out using radio-frequency (rf) spectroscopy detected with resonant excitation Stark ionization spectroscopy (RESIS). Intervals separating L = 9 to L = 15 levels have been measured, and the results analyzed with the long-range effective potential model. The dipole polarizability of Th{sup 4+}is determined to be {alpha}{sub D} = 7.720(7) a.u. The quadrupole polarizability is found to be 21.5(3.9) a.u. Both measurements represent significant tests of a priori theoretical descriptions of this highly relativistic ion.
Wavelengths, line strengths, and transition rates are calculated for the multipole (E1, M1, E2, M2, E3, and M3) transitions between the excited 6s{sup 2}6p{sup 5}nl and 6s6p{sup 6}nl states and the ground 6s{sup 2}6p{sup 6} state in Ac{sup 3+}, Th{sup 4+}, and U{sup 6+} Rn-like ions. Relativistic many-body perturbation theory (RMBPT), including the Breit interaction, is used to evaluate energies and transition rates for multipole transitions in these hole-particle systems. The RMBPT method agrees with multiconfigurational Dirac-Fock (MCDF) calculations in lowest order, includes all second-order correlation corrections, and includes corrections from negative-energy states. The calculations start from a [Xe]4f{sup 14}5d{sup 10}6s{sup 2}6p{sup 6} Dirac-Fock potential. First-order perturbation theory is used to obtain intermediate-coupling coefficients, and second-order RMBPT is used to determine the matrix elements. Evaluated multipole matrix elements for transitions from excited states to the ground states are used to determine the line strengths, transition rates, and multipole polarizabilities. This work provides a number of yet unmeasured properties of these actinide ions for various applications and for benchmark tests of theory and experiment.
The nuclei {sup 230}U and {sup 232}U were populated in the compound nucleus reactions {sup 232}Th({alpha},6n) and {sup 232}Th({alpha},4n), respectively. Gamma rays from these nuclei were observed in coincidence with a recoil detector. A comprehensive set of in-band E2 transitions were observed in the lowest lying negative-parity band of {sup 232}U while one E2 transition was also observed for {sup 230}U. These allowed B(E1;I{sup -{yields}}I{sup +}-1)/B(E2;I{sup -{yields}}I{sup -}-2) ratios to be extracted and compared with systematics. The values are similar to those of their Th and Ra isotones. The possibility of a tetrahedral shape for the negative-parity U bands appears difficult to reconcile with the measured Q{sub 2} values for the isotone {sup 226}Ra.
Reflection asymmetric relativistic mean-field theory is used to investigate the shape evolution for even-even Th isotopes. The calculated deformations, matter density distributions, and potential energy surfaces demonstrate clearly the shape evolution from spherical to octupole deformed. Especially, it is shown that Th isotopes suffer two types of shape transition when the neutron number increases from N=126 to N=156. One is from spherical to octupole deformed around N=134, and another is from octupole to quadrupole deformed around N=150.
Fission properties of proton-induced fission on {sup 232}Th, {sup 237}Np, {sup 238}U, {sup 239}Pu, and {sup 241}Am targets, measured at the Louvain-la-Neuve cyclotron facility at proton energies of 26.5 and 62.9 MeV, are compared with the predictions of the state-of-the-art nuclear reaction code talys. The code couples the multimodal random neck-rupture model with the pre-equilibrium exciton and statistical models to predict fission fragment mass yields, pre- and post-scission neutron multiplicities, and total fission cross sections in a consistent approach. The sensitivity of the calculations to the input parameters of the code and possible improvements are discussed in detail.
No abstract prepared.
Fission fragment angular distributions have been measured for a {sup 9}Be + {sup 232}Th system at four different beam energies around the Coulomb barrier. The experimental results on fission fragment anisotropies have been compared with predictions of the standard statistical saddle-point model (SSPM) and the preequilibrium fission (PEQ) model including projectile ground-state spin. It is observed that both SSPM and the PEQ model fail to reproduce the experimental results, indicating that projectile breakup may affect the fission fragment anisotropies.
No abstract prepared.
Quasielastic excitation function measurement has been carried out for the {sup 4}He + {sup 232}Th system at {theta}{sub lab}=160 deg. with respect to the beam direction, to obtain a representation of the fusion-barrier distribution. Using the present data along with previously measured barrier distribution results on {sup 12}C, {sup 16}O, and {sup 19}F + {sup 232}Th systems, a systematic analysis has been carried out to investigate the role of target and/or projectile structures on fusion-barrier distribution. It is observed that for {sup 4}He, {sup 12}C, and {sup 16}O + {sup 232}Th reactions, the couplings due to target states only are required in coupled-channel fusion calculations to explain the experimental data, whereas for the {sup 19}F + {sup 232}Th system along with the coupling of target states, inelastic states of {sup 19}F are also required to explain the experimental results on fusion-barrier distribution. The width of the barrier distribution shows interesting transition behavior when plotted with respect to the target-projectile charge product for the above systems.
The {alpha}-particle energy spectra have been measured in coincidence with fission fragments over a wide range of relative angles with respect to fragment emission direction in the {sup 11}B (62 MeV) + {sup 232}Th reaction. The {alpha}-particle multiplicity spectra have been fitted with moving source model to extract the precision ({alpha}{sub pre}) and near-scission ({alpha}{sub nse}) components. The present results, along with available data from the literature over a wide range of Z{sup 2}/A and the excitation energy of a compound system, have been analyzed to develop certain global features of the pre- and near-scission emission characteristics. It is seen that {alpha}{sub pre} values when normalized to E{sub CN}{sup 2.3} (E{sub CN} is the compound nucleus excitation energy) show a systematic linearly increasing trend with the {alpha}-particle emission Q value (Q{sub {alpha}}). The fraction of near-scission multiplicity is observed to be nearly the same at around 10% of the total precision multiplicity for all the systems.
Over the last 10 years, a vast campaign of measurements has been initiated to improve the precision of neutron data for the involved key nuclei ({sup 232}Th, {sup 233}Pa and {sup 233}U) of the innovative Th -{sup 233}U cycle. This latter might indeed provide cleaner nuclear energy than the present U-Pu one. New measurements of charge and mass distributions of the fission products have been achieved at the Lohengrin spectrometer of the Inst. Laue-Langevin (ILL) during fall 2010 to complete the experimental data of {sup 233}U(n,f) that exist mainly for light fission fragments. That is why we performed measurements of mass and isotopic yields with a special focus on the heavy fission fragment part. Mass yields were measured by ion counting with an ionization chamber after separation by the Lohengrin spectrometer. Isotopic yields were derived from gamma spectrometry of mass-separated beams using HPGe clover detectors. This paper will present the results of these fission yield measurements along with details on the experimental set-up and the chosen analysis method. (authors)
Design of indirectly heated solid cathode based electron gun (200 kW, 45 kV, 270 degree bent strip type electron gun) has been presented. The solid cathode is made of thoriated tungsten. The solid cathode design has been suitably done to achieve required electron beam cross section. The design approach consists of simulation followed by extensive experimentation. In the design, the effort has been put to reduce the non-uniformity of the heat flux from the filament to the solid cathode to obtain better uniformity of temperature on the solid cathode. Trial beam experiments shows that the modified design achieves one to one correspondence of the solid cathode length and the electron beam length. (author)
In this study, multi-phase silicate-based glass-ceramics were investigated as an alternate waste form for immobilizing non-fissionable products from used nuclear fuel. Currently, borosilicate glass is the waste form selected for immobilization of this waste stream, however, the low thermal stability and solubility of MoO{sub 3} in borosilicate glass translates into a maximum waste loading in the range of 15-20 mass%. Glass-ceramics provide the opportunity to target durable crystalline phases, e.g., powellite, oxyapatite, celsian, and pollucite, that will incorporate MoO{sub 3} as well as other waste components such as lanthanides, alkalis, and alkaline earths at levels 2X the solubility limits of a single-phase glass. In addition a glass-ceramic could provide higher thermal stability, depending upon the properties of the crystalline and amorphous phases. Glass-ceramics were successfully synthesized at waste loadings of 42, 45, and 50 mass% with the following glass additives: B{sub 2}O{sub 3}, Al{sub 2}O{sub 3}, CaO and SiO{sub 2} by slow cooling form from a glass melt. Glass-ceramics were characterized in terms of phase assemblage, morphology, and thermal stability. The targeted phases: powellite and oxyapatite were observed in all of the compositions along with a lanthanide borosilicate, and cerianite. Results of this initial investigation of glass-ceramics show promise as a potential waste form to replace single-phase borosilicate glass.
In 2009, remediation was initiated for a non-operational fuel cycle facility previously used for government contract work located in Windsor, Connecticut, USA. Radiological contaminants consisted primarily of high enriched uranium (HEU). Other radionuclides encountered in relatively minor amounts in certain areas of the clean-up included Co-60, Cs- 137, Ra-226, Th-232 and low enriched uranium (LEU).Between 2009 and the spring of 2011, remediation efforts were focused on demolition of contaminated buildings and removal of contaminated soil. In the late spring of 2011, the last phase of remediation commenced involving the removal of contaminated sediments from portions of a 1,200 meter long gaining stream. Planning and preparation for remediation of the stream began in 2009 with submittal of permit applications to undertake construction activities in a wetland area. The permitting process was lengthy and involved securing permits from multiple agencies. However, early and frequent communication with stakeholders played an integral role in efficiently obtaining the permit approvals. Frequent communication with stakeholders throughout the planning and remediation process also proved to be a key factor in timely completion of the project. The remediation of the stream involved the use of temporary bladder berms to divert surface water flow, water diversion piping, a sediment vacuum removal system, excavation of sediments using small front-end loaders, sediment dewatering, and waste packaging, transportation and disposal. Many safeguards were employed to protect several species of concern in the work area, water management during project activities, challenges encountered during the project, methods of Final Status Survey, and stream restoration. (authors)
Contaminated soils form a large part of the nuclear waste arising from decommissioning activities. The storage and disposal of these large volumes of waste is costly. For this reason techniques which can decontaminate this waste stream to free release levels are economically very interesting. A feasibility study of the possibilities of soil washing to decontaminate such soils was ordered by NIRAS/ONDRAF and performed at Belgoprocess in collaboration with DEC. Initial contamination level and particle size distributions of contaminated soils from three different sources were determined. The main isotopes detected with gamma spectrometry contained in the waste were {sup 241}Am, {sup 137}Cs, {sup 226}Ra, {sup 60}Co and {sup 232}Th. The particle size distribution revealed that more than half of the mass of the quartz sand that makes up the soil has a particle size between 125 and 212 μm. This fraction is less contaminated than the fractions containing smaller particles. However, separation of the fines fraction (< 125 μm) was not enough to achieve the free release limit. Soil attrition was tested as an extra decontamination step for the sand fraction. The removal efficiencies for the different radionuclides contained in the soil were measured. The process conditions were optimized to achieve maximum removal and a treatment method for the secondary waste coming from this process step was determined. The soil washing process was not only performed with water but also with nitric acid to assess the possibilities of a combination of a mechanical and a chemical decontamination process. Reduction efficiencies of 60-80% for the most relevant radionuclides were recorded. (authors)