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DOE OSTI2023

Machine Learning technique for isotopic determination of radioisotopes using HPGe γ-ray spectra

γ-ray spectroscopy is a quantitative, non-destructive technique that may be utilized for the identification and quantitative isotopic estimation of radionuclides. Traditional methods of isotopic determination have various challenges that contribute to statistical and systematic uncertainties in the estimated isotopics. Furthermore, these methods typically require numerous pre-processing steps, and have only been rigorously tested in laboratory settings with limited shielding. Here, in this work, we examine the application of a number of machine learning based regression algorithms as alternatives to conventional approaches for analyzing γ-ray spectroscopy data in the Emergency Response arena. This approach not only eliminates many steps in the analysis procedure, and therefore offers potential to reduce this source of systematic uncertainty, but is also shown to offer comparable performance to conventional approaches in the Emergency Response Application.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Determination of the spins and parities for the $0^+_4$ and $0^+_5$ states in $^{100}Zr$

Two 0 + states at 1294.5 and 1774.0 keV, together with three 2 + and one 4 + levels, were identified or unambiguously spin-parity assigned for the first time in 100 Zr utilizing γ-ray spectroscopy and γ-γ angular correlation techniques with the Gammasphere spectrometer, following the β - decay of neutron-rich, mass separated 100,100m Y isotopes. Comparisons with recent Monte Carlo Shell-Model (MCSM) calculations indicate that these two states are candidates for the bandhead of a sequence in a shape-coexisting spherical minimum predicted to be located around ≈1500 keV. According to the measured relative B(E2) relative transition probabilities, the 0+ 5 state exhibits decay properties which more closely align with those predicted for a spherical shape, while the $0^+_4$ level is suggested to be associated with a weakly-deformed shape similar to one related to the $0^+_2$ state.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Determination of the spins and parities for the $0$$^{+}_{4}$ and $0$$^{+}_{5}$ states in 100 Zr

Two 0 + states at 1294.5 and 1774.0 keV, together with three 2 + and one 4 + levels, were identified or unambiguously spin-parity assigned for the first time in 100 Zr utilizing γ-ray spectroscopy and γ-γ angular correlation techniques with the Gammasphere spectrometer, following the β¯ decay of neutron-rich, mass separated 100,100m Y isotopes. Comparisons with recent Monte Carlo Shell-Model (MCSM) calculations indicate that these two states are candidates for the bandhead of a sequence in a shape-coexisting spherical minimum predicted to be located around ≈1500 keV. According to the measured relative B(E2) relative transition probabilities, the $0$$^{+}_{5}$ state exhibits decay properties which more closely align with those predicted for a spherical shape, while the $0$$^{+}_{4}$ level is suggested to be associated with a weakly-deformed shape similar to one related to the $0$$^{+}_{2}$ state.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

The Primary Interaction Compton Couple algorithm for sorting GRETINA/GRETA interaction points

The Primary Interaction Compton Couple (PICC) algorithm is presented in this work. The algorithm is used to determine the first-interaction-point position for $γ$-ray events in GRETINA. The first-interaction-point position is crucial for in-beam $γ$-ray spectroscopy experiments with fast beams due to the effect of Doppler broadening on the in-beam energy resolution. The development of the algorithm and its performance compared to a tracking algorithm and the Main Interaction assumption is presented. The PICC algorithm is demonstrated with real data to outperform the $γ$-ray energy tracking algorithm used for comparison here and the Main Interaction assumption in first-interaction-point determinations.

GRETINA↗

DOE OSTI2021

Structure of high-lying levels populated in the 96 Y → 96 Zr β decay

The nature of the high-lying final levels of the 96 Y gs β decay, one of the three most important contributors to the high-energy reactor antineutrino spectrum, has been investigated in high-resolution γ-ray spectroscopy following the β decay as well as in a campaign of inelastic photon scattering experiments. The comprehensive approach establishes 1 - levels associated with the Pygmy Dipole Resonance as high-lying final levels in the β decay. Branching ratios extracted from β decay complement photon scattering and allow the absolute E1 excitation strength to be determined for levels populated in both reactions. The combined data represents a comprehensive approach to the wavefunction of the 1 - levels below the Qβ value, which are investigated in the Quasiparticle Phonon Model. The calculations reveal that the components populated in β decay contribute only with small amplitudes to the complex wavefunction of these 1 - levels. A comparison of the β decay results to data from total absorption γ -ray spectroscopy demonstrates a good agreement between both measurements.

Pygmy dipole resonance↗

DOE OSTI2023

Templates of expected measurement uncertainties for neutron-induced capture and charged-particle production cross section observables

This paper provides a template of expected uncertainties and correlations for measurements of neutron-induced capture and charged-particle production cross sections. Measurements performed in-beam include total absorption spectroscopy, total energy detection, γ -ray spectroscopy, and direct charged-particle detection. Offline measurements include activation analysis and accelerator mass spectrometry. The information needed for proper use of the datasets in resonance region and high energy region evaluations is described, and recommended uncertainties are provided when specific values are not available for a dataset.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

237 Np Fission Spectrum Cumulative Fission Product Yield Measurement Using Godiva IV Critical Assembly

Precise integral measurement of fast neutron-induced fission product yields for various actinides is of high interest for applied nuclear science. The goal of this effort is to improve uncertainties in fission product yield values of 237 Np. Fission was induced in a NpO 2 (NO 3 ) target using the Godiva IV critical assembly in burst mode. The irradiated sample was transferred to a high-resolution γ-ray detection setup within 50 minutes. γ-ray list mode data was collected from 50 minutes to 1 week after the irradiation. γ-ray spectroscopy was performed to analyze the time dependent γ-ray yields using an automated peak search algorithm to identify isotopes by their decay γ-ray energy and half-life. Finally, the initial activity for each isotope identified was used to calculate their fission product yield.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

239 Pu Fission Spectrum Cumulative Fission Product Yield Measurement Using Godiva IV Critical Assembly

Precise integral measurement of fast neutron-induced fission product yields for various actinides is of high interest for applied nuclear science. The goal of this effort is to improve uncertainties in fission product yield values of 239 Pu. Fission was induced in a pure 239 Pu (>99%) target using the Godiva IV critical assembly in burst mode. Further, the irradiated sample was transferred to a high-resolution γ-ray detector within 45 minutes. γ-ray list mode data was collected from 45 minutes to 1 week after the irradiation. γ-ray spectroscopy was performed to analyze the time dependent γ-ray yields using an automated peak search algorithm to identify isotopes by their decay γ-ray energy and half-life. The initial activity for each isotope identified was used to calculate their fission product yield.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Development of a rapid-transit system for precision nuclear physics measurements

A Rapid Belt-driven Irradiated Target Transfer System, named RABITTS, was developed for use at the Triangle Universities Nuclear Laboratory. This system allows for cyclic activation with neutron or photon beams, and measurement of reaction products using γ-ray spectroscopy. Both a 1 meter and 10 meter transfer system have been developed with transit times as low as 0.4 and 1.0 seconds, respectively. The systems are deployed at the tandem accelerator laboratory for use with monoenergetic neutron beams, and at the High-Intensity γ-ray Source facility for activation using photon beams. A detailed characterization of the systems’ performance and sensitivity is presented. In order to produce the highest accuracy cross-section data, a model for calculating corrections to cyclic activation with variable beam flux is developed and presented. We have commissioned these systems by measuring 197m Au, where we report a measured half-life of 7.73 ± 0.05 s and a 197 Au(n, n') 197m Au isomer production cross of 628 ± 28 mb at neutron energy E n = 2.0 MeV. In addition, we measured 90m Zr, where we report a measured half-life of 799.7 ± 8.0 ms and a 90 Zr(n, n') 90m Zr isomer production cross of 180 ± 12 mb at E n = 4.6 MeV. Furthermore, these measured half-lives are in excellent agreement with the evaluated values and the cross-section measurements are performed at previously unmeasured incident neutron energies.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2021

New approach to precisely measure γ-ray intensities for long-lived fission products, with results for the decay of 95 Zr

For many fission products, the rays emitted following decay provide an easily-detectable signature that can be used to identify their quantities and distributions in a sample. As a result, γ-ray spectroscopy is often exploited to study fission-product yields, provided sufficiently accurate information on the γ-ray intensity is available. However, in many cases, the uncertainties in the existing nuclear data are large enough that they compromise the precision achievable for modern experiments and applications. To address this need, we have developed a new experimental method that is well suited to precisely measure absolute γ-ray intensities in the β decay of long-lived fission products. The approach involves the production of a radiopure sample by implantation of a mass-separated ion beam from the CAlifornium Rare Isotope Breeder Upgrade (CARIBU) facility on a thin carbon foil. The emitted β-decay radiation is detected with a 4π gas proportional counter and a meticulously efficiency-calibrated high-purity germanium (HPGe) detector. As a first measurement to demonstrate the approach, we studied the absolute γ-ray intensities of the strongest transitions following the β decay of 95 Zr and its decay-daughter 95 Nb, and determined them to fractional precisions of better than 1–2%. In addition, with a larger sample of activity produced through neutron irradiation of an isotopically-enriched Zr foil, we performed a high-precision measurement of the relative γ-ray intensities following the decay of 95 Zr with just the HPGe detector. Here, the sample-production method at CARIBU and the coincidence detection approach demonstrated here can be applied to study fission products with half-lives longer than a day, which includes isotopes important not only for nuclear-energy and national-security applications, but also for medical-isotope research and environmental monitoring.

4π↗

DOE OSTI2023

First Evidence of Axial Shape Asymmetry and Configuration Coexistence in Zn 74 : Suggestion for a Northern Extension of the N = 40 Island of Inversion

The excited states of N=44 74 Zn were investigated via γ-ray spectroscopy following 74 Cu β decay. By exploiting γ-γ angular correlation analysis, the 2$_2^+$, 3$_1^+$, 0$_2^+$, and 2$_3^+$ states in 74 Zn were firmly established. The γ-ray branching and E2/M1 mixing ratios for transitions deexciting the 2$_2^+$, 3$_1^+$, and 2$_3^+$ states were measured, allowing for the extraction of relative B(E2) values. In particular, the 2$_3^+$→0$_2^+$ and 2$_3^+$→4$_1^+$ transitions were observed for the first time. Here the results show excellent agreement with new microscopic large-scale shell-model calculations, and are discussed in terms of underlying shapes, as well as the role of neutron excitations across the N=40 gap. Enhanced axial shape asymmetry (triaxiality) is suggested to characterize 74 Zn in its ground state. Furthermore, an excited K=0 band with a significantly larger softness in its shape is identified. A shore of the N=40 "island of inversion" appears to manifest above Z=26, previously thought as its northern limit in the chart of the nuclides.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

Absolute efficiency response of the γ-ray spectrometer GRETINA for high-energy γ rays up to 6 MeV

GRETINA (Gamma-Ray Energy Tracking In-beam Nuclear Array), a state-of-the-art γ-ray tracking spectrometer, has been instrumental in advancing nuclear structure studies, particularly in experiments using fast beams of rare isotopes where the γ rays emitted in flight are subject to large Doppler shifts. This work presents an experimental determination of the γ-ray detection efficiency of GRETINA at energies up to 6 MeV. The high-energy γ rays originated from states that were populated in nucleon-removal reactions from a projectile beam at an intermediate beam energy of about 85 MeV/nucleon. Utilizing γ-γ coincidences, efficiency values were extracted in-beam and translated into a source efficiency at rest employing GEANT4 Monte Carlo simulations. A systematic discrepancy in the efficiency of the forward-positioned detectors was identified which is attributed to specific dead-time effects caused by high-energy light-particle events prevalent at forward angles, generating signals in the Ge crystals that saturate the preamplifier’s first stage. Furthermore, this study provides refined efficiency benchmarks for in-beam experiments, improving the accuracy of quantitative γ-ray spectroscopy analyses with GRETINA and GRETA (Gamma Ray Energy Tracking Array) in the future.

GRETINA↗

DOE OSTI2023

Intruder configurations in 29 Ne at the transition into the island of inversion: Detailed structure study of 28 Ne

Detailed γ-ray spectroscopy of the exotic neon isotope 28 Ne has been performed for the first time using the one-neutron removal reaction from 29 Ne on a liquid hydrogen target at 240 MeV/nucleon. Based on an analysis of parallel momentum distributions, a level scheme with spin-parity assignments has been constructed for 28 Ne and the negative-parity states are identified for the first time. The measured partial cross sections and momentum distributions reveal a significant intruder p-wave strength providing evidence of the breakdown of the N=20 and N=28 shell gaps. Only a weak, possible f-wave strength was observed to bound final states. Large-scale shell-model calculations with different effective interactions do not reproduce the large p-wave and small f-wave strength observed experimentally, indicating an ongoing challenge for a complete theoretical description of the transition into the island of inversion along the Ne isotopic chain.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Precise measurements of the γ -ray intensities following the β decay of Ce 144 and Nd 147

For many fission products, the γ rays emitted following β decay provide an easily detectable signature that can be used to identify their quantities and distributions in a sample. As a result, γ-ray spectroscopy is often exploited to study fission-product yields, provided sufficiently accurate information on the γ-ray intensities is available. Further, in many cases, the uncertainties in the existing nuclear data are large enough that they compromise the precision achievable for modern experiments and applications. In this paper, we present high-precision results for the absolute γ-ray emission intensities for the most intense transitions in the β decays of 144 Ce and 147 Nd. We measured these intensities to ≲1% accuracy by producing radiopure samples with fission-product beams at CARIBU and detecting the emitted radiation with a 4⁢πβ counter and a meticulously efficiency-calibrated high purity germanium detector at Texas A&M University.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Level structure of the T z = –1 nucleus 34 Ar and its relevance for nucleosynthesis in ONe novae

The 24 Mg+ 12 C fusion reaction was used to perform a detailed γ-ray spectroscopy study of the astrophysically important nucleus 34 Ar. In particular, an experimental setup, coupling the advanced γ-ray tracking array GRETINA with the well-established Argonne fragment mass analyzer (FMA), was employed to obtain excitation energies and spin-parity assignments for excited states in 34 Ar, both above and below the proton separation energy. For the first time, an angular distribution analysis of in-beam γ rays from fusion-evaporation reactions, using a tracking array, has been performed and Coulomb energy differences of analog states in the T = 1, A = 34 mirror system, explored from 0 to 6 MeV. Lastly, we present a comprehensive discussion of the astrophysical 33 Cl(p,γ) stellar reaction rate, together with implications for the identification of nova presolar grains from sulfur isotopic abundances.

20 ≤ A ≤ 38↗

DOE OSTI2020

Determination of γ-ray branching ratios for ⁹⁵Zr and ¹⁴⁷Nd

For many fission products, the γ rays emitted following decay provide an easily-detectable signature that can be used to identify their quantities and distributions in a sample. As a result, γ-ray spectroscopy is often exploited to study fission-product yields (FPYs), provided sufficiently accurate information on the γ-ray branching ratio is available. However, in many cases, the uncertainties in the existing nuclear data are large enough that they compromise the precision achievable for modern experiments and applications. To address this need, we have developed a new experimental method that is well suited to precisely measure the γ-ray branching ratios in the decay of long-lived fission products. The approach involves the production of a radiopure sample by implantation of a mass-separated ion beam from the CAlifornium Rare Isotope Breeder Upgrade (CARIBU) facility on a thin carbon foil. The emitted β -decay radiation is detected with a 4π gas proportional counter and a meticulously efficiency-calibrated high-purity germanium (HPGe) detector. As a first measurement to demonstrate the approach, we studied the γ-ray branching ratios of the strongest transitions following the decay of ⁹⁵Zr and decay-daughter ⁹⁵Nb and determined these branching ratios to fractional precisions of 1%. We then applied this approach to determine the γ-ray branching ratios for the β decay of ¹⁴⁷Nd. The results for the γ-ray branching ratios are presented here and compared to previous results and evaluations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Dipole response in Te 128 , 130 below the neutron threshold

Numerous studies of the ground-state decay of the pygmy dipole resonance (PDR) have been carried out in the past. However, data on the decay of the PDR to low-lying excited states is still very scarce due to limitations of the sensitivity to weak branching transitions of experimental setups. Here, we present a detailed examination of the low-energy dipole response of 128 Te and 130 Te below their neutron separation thresholds of 8.8 and 8.5 MeV, respectively. Photonuclear reactions with the subsequent γ-ray spectroscopy of the decay channel with continuous-energy bremsstrahlung at varying endpoint energies and linearly polarized quasimonochromatic γ-ray beams with energies ranging from 2.7 to 8.9 MeV in steps of roughly 250 keV were used for probing the decay behavior of the low-energy dipole response in 128Te and 130Te. In addition, (γ,γ' γ") reactions were used to study the population of low-lying states of 128 Te. Spin-parity quantum numbers and reduced transition probabilities are determined for individual photo-excited states. The analysis of average decay properties for nuclear levels in narrow excitation-energy bins enable the extraction of photoabsorption cross sections, average branching ratios to the $2$$^{+}_{1}$ state, and the distinction between E1 and M1 transitions to the ground state and to the $2$$^{+}_{1}$ state accounting for resolved and unresolved transitions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

Isospin symmetry holds beyond the proton drip line: First observation of excited states in 55Cu

Isospin symmetry, combined with shell-model description, has long been successful in reproducing nuclear structure and predicting mirror energy differences. However, these descriptions have been primarily limited to mirror nuclei with well-bound ground states. As one approaches the proton drip line, coupling to the continuum becomes important. Despite this, little is known about medium-mass nuclei at the drip line. Here we report the measurement of the excitation energies of several unbound states in a nucleus beyond the proton drip line, 55Cu, performed via γ-ray spectroscopy at the Radioactive Isotope Beam Factory (RIKEN). Several low-lying yrast states are observed to decay predominantly by γ-ray emission. In contrast, the state–predicted to be strongly populated in the one-proton knockout reaction–is notably absent, suggesting that it decays primarily via prompt proton emission. We show that even for such an unbound system, shell-model calculations based on a harmonic oscillator potential reproduce the observed mirror energy differences remarkably well in all the observed states. Based on this result, we propose that a general pattern might emerge where, in medium-mass systems at the proton drip line, the stronger Coulomb barrier together with the centrifugal barrier effectively confines the wave functions, so that the shell model is able to describe low-lying states, enabling accurate predictions of mirror energy differences between isobaric analogue states.

Pigliapoco, S [Dipartimento di Fisica e Astronomia↗