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At least 91 records · Page 5

Weak decays in superheavy nuclei

Superheavy nuclei represent the extreme atoms and nuclides known at the limit of mass and charge. The observed superheavy nuclei are all proton-rich; they decay primarily by emitting 𝛼 particles and by fission with a possible small electron capture (EC) branch. Here, due to the huge atomic numbers and associated relativistic effects, EC decays of superheavy systems are expected to differ from what is known in lighter nuclei. In this letter, using the quantified relativistic nuclear density functional theory and the quasiparticle random-phase approximation with the interaction optimized to experimental EC/𝛽 ± -decay half-lives, and Gamow-Teller resonance energies, we study the EC/𝛽 ± -decays in 𝑍=101–118 nuclei. Both allowed (1 + ) and first-forbidden (0 − ,1 − and 2 − ) transitions are considered. We show that the first-forbidden 1 − transitions dominate the decay rates in almost all studied nuclei. For proton-rich nuclei, EC dominates over 𝛽 + decay. Based on calculations with two relativistic energy density functionals, we identify 45 candidate nuclei in which a competition between weak decays and 𝛼 decay and spontaneous fission is expected.

A ≥ 220↗

Enhanced detection limits for radiokrypton analysis

In this paper, we present a method for improving detection limits of Atom Trap Trace Analysis for the krypton radioisotopes 85 Kr and 81 Kr. For the case of 85 Kr this work demonstrates that systematic use of isotopically depleted gas for calibration and extended conditioning of the instrument results in a detection limit of 900 85 Kr atoms per 11 μl of Kr gas, equivalent to a 85 Kr/Kr isotopic abundance of 3 x 10 -15 . This improvement of roughly two orders of magnitude over previously reported limits will help to expand the reach of radiokrypton dating towards longer age ranges where most of the radioisotopes have decayed. Additionally, the method offers an opportunity to investigate radiokrypton production via spontaneous fission within naturally occurring minerals to understand potential underground production of these isotopes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

The calculation of light element impurity (α, n) yield curves in a PuO 2 matrix and associated specific yield coefficients: Influence of the reaction cross sections

Most of the Pu separated from irradiated commercial nuclear fuel is stored as PuO 2 . The primary quantitative nondestructive measurement technique used to verify the amount of Pu in storage containers is passive neutron correlation counting. An important physical property of the oxide material is the ratio, α, of the rate of (α, n) neutrons produced inside the item to the rate of neutrons produced by spontaneous fission. This ratio influences the precision of the correlated counting method and affects the interpretation of the data because of how it changes both the primary total neutron production rate and the rate of induced fission events taking place inside the item. In addition to the main O(α, n) contribution, additional contributions come from α-particle interactions with light element impurities that are inevitably present. In this work, we calculate specific (α, n) yield coefficients, expressed in units of neutrons per second per gram of α-emitting nuclide per part per million by mass of the specified impurity element distributed in a pure PuO 2 matrix, for some key α-emitting actinides commonly present in reprocessed Pu ( 238–242 Pu+ 241 Am). These coefficients are directly applicable to nuclear safeguards verification work in which the α ratio is often calculated from the Pu-isotopic composition and chemical information obtained by other means. Further, they also provide a convenient up-to-date reference set against which values generated by other methods can be compared. Results are presented for impurities with atomic number from 3 to 17 inclusive, plus K and Fe. In most cases, these coefficients are not expected to change by more than 5%–10% at any time in the future. However, as new data become available, changes as large as 20% may be needed for some targets (e.g., F). The present yield calculations are limited by the general shortage of quality experimental total (α, n) reaction cross section data, which, together with unexplained variation between determinations, means that an objective and coherent evaluation is not possible. The situation is even less satisfactory for the partial differential cross section needed to calculate neutron spectra.

(𝛼, n) reactions↗

252 Cf yield calibration method for nuclear material accountancy and safeguards practitioners

Californium-252 is an isotope commonly encapsulated as a physically small but strong spontaneous fission neutron source for applications in industry, academia, and research. Within the nuclear safeguards community, a well-characterized 252 Cf source is often used as an accessible alternative for plutonium in calibrations measurements, which require the absolute source strength. Current methods of source strength quantification can provide an accurate estimate, approximately 1% uncertainty under optimal conditions, but are typically costly and time consuming. An alternative method was developed to determine 252 Cf source strength using passive neutron correlation counting (PNCC). The PNCC method enables institutions and facilities to perform 252 Cf source calibration measurements in-house using detection systems that are common within the nuclear safeguards community. This novel method was previously successfully demonstrated using neutron multiplicity well counters. However, the previous evaluation utilized detection systems with high neutron detection efficiencies, greater than 60%. The purpose of the current study is to extend the previous evaluation and demonstrate the feasibility of the PNCC 252 Cf calibration method for suite of coincidence counters with lower neutron detection efficiencies, between 15% and 35%, which are more commonly encountered in the field, as well as to provide a step-by-step guide to using the method. The neutron source used in this evaluation was previously certified by the National Institutes of Science and Technology (NIST), which provides a reference for the accuracy of the PNCC method. In conclusion, the present source yield calculations demonstrate excellent agreement with a NIST calibration technique and achieve a standard uncertainty below the target 1%.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Use of a deuterium-deuterium neutron generator for the Add-A-Source waste matrix correction technique

Neutron generators offer an alternative to radioactive sources in the application of active techniques for nondestructive assay of nuclear materials. The Add-A-Source technique has enabled improvements in the ability to accurately measure waste bearing nuclear materials by measuring and correcting for the non-nuclear matrix effect. The technique has historically been performed with a Cf-252 spontaneous fission source. Here, in this work, we have demonstrated the use of a Deuterium-deuterium neutron generator in place of the Cf-252 source. A DD generator enables operational advantages and allows the simplification of the instrument design, while offering equivalent corrective performance as a Cf-252 source.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Derivation of at-birth neutron energy distribution of americium-beryllium source based on ISO8529 spectral data

In many practical applications, the accuracy of neutron transport calculations depends on an estimate of the energy distribution provided in the source definition. While the energy distribution of neutrons emitted by spontaneous fission sources is well-defined, the spectra of neutrons produced in (α,n) reactions in compound mixtures, such as americium-beryllium (AmBe), depend on the microstructural properties of the source material, which may vary. Although the energy of neutrons produced in nuclear reactions can be calculated from first principles, such computations require detailed knowledge of the key characteristics of the source material, which are often unknown. Here, this study focuses on deriving the at-birth neutron energy distribution for an AmBe source by applying reverse transport calculations to the externally measured high-precision spectrum recommended in the latest revision of the international standard. The derived at-birth spectrum was validated through indirect energy-sensitive neutron emission rate measurements of AmBe sources calibrated at national primary metrology institutions. The resulting at-birth neutron energy distribution serves as essential input data for radiation transport modeling, providing a validated spectrum for broader experimental and computational applications.

AmBe↗

Coexistence of octupole deformation and beta and gamma vibrational bands in 148 Ce

From γ-γ-γ and γ-γ-γ-γ coincidence studies of spontaneous fission of 252 Cf, new high spin states in 148 Ce were identified. The octupole bands with s = +1 and s = -1 are expanded with spins with 28 + and 18 - , respectively. Importantly, a 1γ vibrational band has been established up to 14 + and a 1β vibrational band up to 6 + . The levels in γ and β bands in 148 Ce are compared systematically to those in neighboring 150 Nd and 152 Sm isotones. Further, this comparison informs the role of deformation and shape transition in this mass region. New 3 - and 5 - members of the s = +1 octupole band were observed.

148Ce↗

Gallium oxide (Ga2O3) as a radiation detector distinguishing neutrons and gammas

Gallium oxide (Ga2O3) is a promising ultrawide bandgap semiconductor for radiation detection with the potential of integrating electronic and scintillation functions within a single crystal device. This study establishes the scintillation response of β-Ga2O3 gamma irradiation from yttrium-88 (88Y). Then, californium-252 (252Cf) is used as a spontaneous fission source of mixed neutron and gamma radiation field to measure scintillation signals. Pulse shape discrimination and constant fraction discrimination techniques were used to separate neutron and gamma interaction events. Further investigation indicates that the prompt temporal responses of β-Ga2O3 for gammas and neutrons may enable discrimination of the two by prompt pulse fitting methods, focused around the initial peak. For gamma irradiation, we observed a rise time (τr) of 2.1 ns, decay time (τd) of 9.5 ns, and a full width at half maximum (FWHM) of 6.2 ns. For neutrons, it showed a τr of 2.3 ns, a τd of 12.1 ns, 9.4 ns FWHM, and reduced peak intensity. A diamond detector exhibited a more symmetrical τr and τd for both gamma and neutron signals and therefore is less effective at discriminating between the two by this method. This draws attention to β-Ga2O3’s ability to distinguish neutron and gamma particles. These findings showcase Ga2O3’s potential as a next-generation semiconductor for applications in nuclear safety and medical imaging, where precise discrimination between neutron and gamma interactions is essential.

Valdes, D. J. (ORCID:0000000304373720)↗

Space-Dependent Calculation of the Multiplicity Moments for Shells With the Inclusion of Scattering

In recent work, we extended the methodology of multiplicity counting in nuclear safeguards by elaborating the one-speed stochastic transport theory of the calculation of the so-called multiplicity moments, i.e., the factorial moments of the number of neutrons emitted from a fissile item, following a source event from an internal neutron source [spontaneous fission and (α; n) reactions]. Calculations were made for solid spheres and cylinders, with the source being homogeneously distributed within the item. Recent measurements of the Rocky Flats Shells during the Measurement of Uranium Subcritical and Critical (MUSIC) campaign conducted by Los Alamos National Laboratory and assisted by the University of Michigan inspired us to extend the model to spherical shell geometry with a point source in the middle of the central cavity. Comparison of the calculated results with the experimental ones indicated that accounting for fission as the only neutron reaction (the standard procedure in the point model, adapted also in our work so far) was not sufficient for reaching good agreement with measurements. The model was therefore extended to include elastic scattering into the one speed formalism, whereas the effect of inelastic scattering was accounted for in an empirical way. After these extensions, good agreement was found between the calculated and the measured values. The paper describes the extension of the theory and provides concrete quantitative results.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Multiphysics Analyses of the Protected and Unprotected Loss of Forced Cooling Accidents in the HTR-PM

Here, we present the multiphysics simulation results for the protected pressurized and depressurized loss of forced cooling (PLOFC and DLOFC) events in the High-Temperature gas-cooled Reactor--Pebble-bed Module (HTR-PM) equilibrium core using the Griffin-Pronghorn coupled code system. Additionally, this paper discusses the strategy for estimating the spontaneous fission neutron source needed for unprotected events and re-criticality calculations. The solutions of the protected PLOFC and DLOFC events were verified against similar solutions obtained for temperature evolutions from the open literature. Both the average and maximum pebble surface temperatures behaved as expected during the DLOFC and remained below 1800 K. The PLOFC results are highly dependent on the ability to resolve the natural circulation in the core, which is impacted by the mesh resolution in Pronghorn. Furthermore, we present the results of the unprotected DLOFC transient to predict the timing of the re-criticality event, which occurred 47 hours after the onset of the transient, and the new steady-state power of 1.3 MW.

42 - ENGINEERING↗

Fingerprints of Triaxiality in the Charge Radii of Neutron-Rich Ruthenium

We present the first measurements with a new collinear laser spectroscopy setup at the Argonne Tandem Linac Accelerator System, utilizing its unique capability to deliver neutron-rich refractory metal isotopes produced by the spontaneous fission of 252 Cf. We measured isotope shifts from optical spectra for nine radioactive ruthenium isotopes 106–114 Ru, reaching deep into the mid-shell region. The extracted charge radii are in excellent agreement with predictions from the Brussels-Skyrme-on-a-Grid models that account for the triaxial deformation of nuclear ground states. We show that triaxial deformation impacts charge radii in models that feature shell effects, in contrast to what could be concluded from a liquid drop analysis. This indicates that this exotic type of deformation should not be neglected in regions where it is known to occur, even if its presence cannot be unambiguously inferred through laser spectroscopy.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Investigation of the 244 Pu ⁢( 48 Ca,𝑥⁢𝑛) 292−𝑥 Fl reaction with the LBNL SHREC detector: Investigation of decay chains of isotopes of flerovium (𝑍=114)

The 244 Pu ⁢( 48 Ca,𝑥⁢𝑛)⁢ 292−𝑥 Fl reaction was investigated at Lawrence Berkeley National Laboratory’s 88 Inch Cyclotron using the Berkeley Gas-filled Separator (BGS), the newly installed Superheavy Recoil detector, along with an upgraded digital electronics and data acquisition system. Seven decay chains were observed starting with an evaporation residue, followed by a single 𝛼 decay and a spontaneous fission. The decay characteristics of these seven decay chains led to an assignment to 288 Fl , the product of the 4⁢𝑛 reaction channel. Two additional chains were (tentatively) assigned to the decay of the 3⁢𝑛 exit channel, 289 Fl . Cross sections for the 4⁢𝑛 and 3⁢𝑛 exit channels were 𝜎 prod =6.7⁢($^{36}_{25}$) pb and 𝜎 prod =1.6⁢($^{22}_{11}$) pb, respectively. Another decay chain, tentatively assigned to the 5⁢𝑛 exit channel through the 48 Ca + 244 Pu reaction or the 3⁢𝑛 exit channel of the 48 Ca + 242 Pu reaction, was also detected. Detailed information regarding the observed decay chains and their nuclear structure aspects is discussed, along with the performance of the BGS and the new detection system.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

First observation of excited states in the 154 Ce 96 nucleus: Rigid rotation at Z = 58

We report new analysis of the data from measurements of γ radiation following spontaneous fission of 248 Cm and 252 Cf, performed using Eurogam2 and Gammashpere arrays, respectively, has revealed, for the first time, excited states in the neutron-rich nucleus, 154 Ce 96 . Using these fission data we have also improved uncertainties on γ-ray energies in the ground-state bands of several neutron-rich nuclei of the A≈150 mass region. The improved data provided precise systematics of the E exc (4+)/E exc (2+) ratio in the region, which indicates that in the Ce isotopic chain the rigid-rotation limit is reached at the neutron number N=96, two neutrons “later” than in the chain of Nd isotopes. The new results suggest the involvement of the proton 9/2 + [404] extruder orbital in generating nuclear deformation in the A≈150 region, analogous to the known role played by the neutron 11/2 – [505] extruder in this region. The catalytic-type action of both extruders is discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Pseudospin-doublet bands and Gallagher Moszkowski doublet bands in 100 Y

New transitions in neutron-rich 100 Y have been identified in a 9 Be + 238 U experiment with mass and Z gates to provide full fragment identification. These transitions and high spin levels of 100 Y have been investigated by analyzing the high statistics γ–γ–γ and γ–γ–γ–γ coincidence data from the spontaneous fission of 252 Cf at the Gammasphere detector array. Two new bands, 14 new levels, and 23 new transitions have been identified. The K π = 4 + new band decaying to a 1s isomeric state is assigned to be the high-K Gallagher-Moszkowski (GM) partner of the known K π = 1 + band, with the π5/2[522]Ⓧν3/2[411] configuration. This 4 + band is also proposed to be the pseudospin partner of the new K π = 5 + band with a 5 + π5/2[422] Ⓧ ν5/2[413] configuration, to form a π5/2[422] Ⓧ ν[3125/2,3/2] neutron pseudospin doublet. Here, constrained triaxial covariant density-functional theory and quantal particle rotor model calculations have been applied to interpret the band structure and available electromagnetic transition probabilities and are found to be in good agreement with experimental values.

100Y↗

First experiment at the Super Heavy Element Factory: High cross section of Mc 288 in the Am 243 + Ca 48 reaction and identification of the new isotope Lr 264

Here, we present results of the first experiment aimed at the synthesis of Mc isotopes in the 243 Am+ 48 Ca reaction performed at the new gas-filled separator DGFRS-2 online to the new cyclotron DC280 at the Super Heavy Element Factory at JINR. Fifty-five new decay chains of 288 Mc and six chains assigned to 289 Mc were detected. The α decay of 268 Db with an energy of 7.6–8.0 MeV, half-life of 16$^{+6}_{-4}$h, and a branch of 55$^{+20}_{-15}$% was registered for the first time, and a new spontaneously fissioning isotope 264 Lr with a half-life of 4.9$^{+2.1}_{-1.3}$h was identified. The cross section for the 243 Am( 48 Ca,3n) 288 Mc reaction was measured to be 17.1$^{+6.3}_{-4.7}$ pb, which is the largest value for the known superheavy nuclei at the island of stability.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Properties of the 256 Db decay chain

Experiments were performed at Lawrence Berkeley National Laboratory's 88-Inch Cyclotron Facility to study the decays of neutron-deficient dubnium isotopes. These isotopes were produced in the 206 Pb( 51 V, xn) 255,256 Db reaction, and excitation functions were measured. This article reports on the observed properties of the 256 Db decay chain. The produced 256 Db nuclei were separated from unreacted-beam material and reaction byproducts with the Berkeley Gas-filled Separator (BGS) before being implanted into a double-sided silicon strip detector at the BGS focal plane. Decay properties of 256 Db and its daughters were then extracted from the analysis of correlations between implanted Db nuclei with α decay chains and spontaneous fission (SF) events. In total, 86 decay chains and 38 SF events were observed, giving increased statistics as compared to previous studies. In conclusion, improved decay data are presented for 256 Db and its daughter isotopes 252 Lr, 252 No, 248 Md, 248 Fm, 244 Es, and 244 Cf.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Coexistence of Reflection Asymmetric and Symmetric Shapes in $^{144}\mathrm{Ba}$

Level structures in the neutron-rich $^{144}\mathrm{Ba}$ nucleus have been reinvestigated by measuring prompt gamma rays in the spontaneous fission of $^{252}\mathrm{Cf}$. The previous $s = +1$ octupole band structure with reflection asymmetric shape has been expanded, and a side quadrupole band structure based on a $3^+$ state with reflection symmetric shape is identified. Thus, the results show the coexistence of reflection asymmetric and symmetric shapes in $^{144}\mathrm{Ba}$. This is a first identification of such a shape coexistence structure in a nuclear structure. Finally, the other structural characteristics are discussed.

144Ba↗

SOURCES4D

SOURCES is a code for computing neutron source rates and spectra from spontaneous fission (including delayed neutrons) and (alpha,n) reactions in homogeneous materials and (alpha,n) reactions in single-interface and two-interface geometries. SOURCES is a Los Alamos National Laboratory (LANL) code that is written in FORTRAN and distributed through the Radiation Safety Information Computation Center (RSICC). LANL’s last release of SOURCES to RSICC was SOURCES4C in 2002. This disclosure covers the latest version of SOURCES, SOURCES4D. This version adds sensitivity capabilities for (alpha,n) sources in homogeneous materials. Specifically, SOURCES4D writes new output that can be used to calculate, in post-processing, first and second derivatives of the (alpha,n) source rate density and spectrum with respect to nuclide densities in a homogeneous material and first derivatives of the (alpha,n) source rate density and spectrum with respect to nuclide stopping powers and (alpha,n) cross sections (nuclear data). These derivatives are useful for uncertainty quantification, predictive modeling, and other applications in neutron transport problems.

Favorite, Jeffrey A.↗