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At least 91 records · Page 5

Internal-Gelation Production of Uranium Oxide Sol-Gel Particles for Forensic Applications

The purpose of this project was to develop and demonstrate a novel method for the production of uranium oxide microsphere particles with tunable chemical compositions via a sol-gel process using a 3D-printer setup. These particles can serve several purposes in research and development as a forensic training tool or as standard reference materials. A key component of the project was to demonstrate the ability to control physical and chemical parameters of the particles created. First, we demonstrated the ability to employ an internal gelation sol-gel process to create individual uranium oxide particles. The particles were successfully dispensed using a unique 3D-printing setup onto a substrate to react and then were collected and thermally processed. A series of temperatures for the annealing process was tested on individual samples to investigate the effect on the sol-gel chemical composition and physical integrity. Next, we demonstrated the ability to control matrix composition of the particles by separately incorporating fission product isotopes as well as Np-237 into the sol-gel solution. It was shown by gamma-ray spectroscopy that these matrix elements were successfully retained during the gelation process. We studied the retention of the elements across a series of annealing temperatures. Additionally, we demonstrated the ability to quantitatively control the isotopic composition of the particles by altering the U-237/U-238 ratio to a controlled value. Finally, X-ray diffraction analysis (XRD) was used to investigate the oxidation state of the sol-gel after annealing at different temperatures.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗

Prototype X-ray and Gamma Detection with Cyclotron Radiation Emission Spectroscopy

Cyclotron radiation emission spectroscopy, or CRES, is a novel approach to measuring the energy of an electron. By trapping a free electron in a high magnetic field, it undergoes cyclotron motion and emits radiofrequency (RF) waves. The frequency of this RF radiation is directly related to the energy of the electron. Because many cycles of the RF emission are recorded, the energy resolution of the CRES system is on the order of a single electron volt. To make a CRES system sensitive to photons, a target gas is used to induce a photoelectric effect, producing the electron that is subsequently trapped. By adding the binding energy of the target atom, the energy of the incident photon may be reconstructed. Using a xenon target gas, photoelectric interactions dominate up to approximately 300 keV, covering not only all atomic shell X-rays of the elements, but many low-lying nuclear states as well, including key transuranic elements related to nuclear security. CRES holds the potential of maintaining single-eV resolution up to this 300-keV range, thereby surpassing current state-of-the-art detectors by a factor of 10-100. The instrumental resolution of the system is limited by the uniformity of the applied magnetic field.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Evidence for an isomeric {pi}½{sup +}[411] state in {sup 183}Ta

We report on the identification of a new isomeric state in Ta populated via the ground-state -decay of Hf. The experiment was performed at the KISS setup at RIKEN, where neutron-rich hafnium isotopes were produced via multi-nucleon transfer (MNT) reactions, followed by laser ionization of hafnium atoms, mass separation, and detection using an electron-gamma coincidence system. Isomeric spectroscopy was carried out by gating on different electron-gamma time correlations. A 459.1 keV -ray transition was identified in delayed spectra, and a half-life of μ was extracted through time-distribution fitting. The 459.1 keV state in Ta is known from previous work and has been assigned a Nilsson orbital configuration of , while a proposed new isomeric state above it is interpreted as a configuration that decays to via a low-energy, unobserved E2 transition. This is consistent with the systematic trends in neighbouring odd-A nuclei and transition rate calculations. Similar content being viewed by others

Doshi, S.↗

Steam-Assisted Ammonolysis of MoO2 as a Synthetic Pathway to Oxygenated δ-MoN

A common route for the synthesis of molybdenum nitrides is through the temperature-programmed reaction of molybdenum oxides with NH3, or ammonolysis. In this work, the role of precursor phase, gas phase chemistry (impact of H2O), and temperature profile on the reaction outcome (700 °C) was examined, which resulted in varying amounts of MoO2, H2MoO5, and the nitride phases—cubic γ (nominally Mo2N) and hexagonal δ (nominally MoN). The phase fraction of the δ phase increased with precursor in the sequence MoO2 > MoO3 > H2MoO5. Steam in the reaction gas also favored the production of δ over γ, but with too much steam, MoO2 was obtained in the product. Synthesis conditions for obtaining nearly phase-pure δ were identified: MoO2 as the precursor, 2% H2O in the gas stream, and a moderate heating rate (3 °C/min). In situ X-ray diffraction provided insights into the reaction pathway. Extensive physico-chemical analysis of the δ phase, including synchrotron X-ray and neutron diffraction, electron microscopy, thermogravimetric analysis, X-ray photoelectron spectroscopy, and prompt gamma activation analysis, revealed its stoichiometry to be MoO0.108(8)N0.892(8)H0.012(5), indicating non-trivial oxygen incorporation. The presence of N/O ordering and an impurity phase Mo5N6 were also revealed, detectable only by neutron diffraction. Notably, a computationally predicted MoON phase (doi: 10.1103/PhysRevLett.123.236402), of interest due to its potential to display a metal-insulator transition, did not appear under any reaction condition examined.

Pandey, Shobhit↗

Identification and time evolution of thionyl chloride (SOCl 2 ) radiolysis products

In this study, innovative solutions are needed to reduce the amount of high-level waste generated by used nuclear fuel recycling strategies to support the widespread adoption of sustainable nuclear fission energy technologies. To this end, a new sulfur chloride-based process has been developed to recycle zirconium alloy-based materials, which make up a significant fraction of high-level radioactive waste. To support the continued development of this process, we present new data on the potential reaction pathways over time of the products arising from the gamma and electron beam radiolysis of neat thionyl chloride (SOCl 2 ). Interrogation of the gamma irradiated liquid by Raman spectroscopy provided more conclusive identification of the SOCl 2 degradation products, specifically sulfur dichloride (SCl 2 ), molecular chlorine (Cl 2 ), sulfur dioxide (SO 2 ), and sulfuryl chloride (SO 2 Cl 2 ). In comparison, the high dose rate (~10 7 Gy s -1 ) electron beam irradiations formed significantly more degradation products. For both cobalt-60 gamma and electron beam irradiations, the observed degradation products were found to evolve as a function of time post-irradiation via the same reaction pathways, with indication of a solvent regeneration mechanism. These findings are fortuitous for process development, as such a mechanism would be beneficial for process longevity and cost effectiveness.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Characterizing hole trap production due to proton irradiation in germanium cross-strip detectors

We present an investigation into the effects of high-energy proton damage on charge trapping in germanium cross-strip detectors with the goal of accomplishing three important measurements. First, we calibrated and characterized the spectral resolution of a spare COSI-balloon detector in order to determine the effects of intrinsic trapping, finding that electron trapping due to impurities dominates over hole trapping in the undamaged detector. Second, we performed two rounds of proton irradiation of the detector in order to quantify, for the first time, the rate at which charge traps are produced by proton irradiation. We find that the product of the hole trap density and cross-sectional area, [nσ] h , follows a linear relationship with the proton fluence, F p , with a slope of (5.4 ± 0.4) x 10 -11 cm/p + . Third, by utilizing our measurements of physical trapping parameters, we performed calibrations which corrected for the effects of trapping and mitigated degradation to the spectral resolution of the detector.

79 ASTRONOMY AND ASTROPHYSICS↗

Isotopic gamma lines for identification of shielding materials

Identifying the constituting materials of concealed objects is crucial in a wide range of sectors, such as medical imaging, geophysics, nonproliferation, national security investigations, and so on. Existing methods face limitations, particularly when multiple materials are involved or when there are challenges posed by scattered radiation and large areal mass. Here we introduce a novel brute-force statistical approach for material identification using high spectral resolution detectors, such as HPGe. The method relies upon updated semianalytic formulae for computing uncollided flux from source of gamma radiation, shielded by a sequence of nested spherical or cylindrical materials. These semianalytical formulae make possible rapid flux estimation for material characterization via combinatorial search through all possible combinations of materials, using a high-resolution HPGe counting detector. An important prerequisite for the method is that the geometry of the objects is known (for example, from X-ray radiography). We demonstrate the viability of this material characterization technique in several use cases with both simulated and experimental data in spherical geometry.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

γIn-beam angular distribution and linear polarization measurements with GRETINA using a simple energy-ordering approach

Angular distribution and linear polarization measurements are powerful tools for inferring the spins and parities of nuclear levels. In this work, the performance of the Gamma-Ray Energy Tracking In-beam Nuclear Array (GRETINA) as a Compton polarimeter was characterized in a fusion-evaporation reaction experiment using a simple energy-ordering approach for the interaction points assigned in the signal decomposition process. A variety of multipolarities and characters for γ-ray transitions in the reaction products 25 Mg, 25 Na, and 22 Ne, formed from fusion-evaporation of an 18 O beam on a 9 Be target, were examined. The experimental angular distributions and linear polarization asymmetries were consistent with predictions using the theoretical formalism accounting for the Lorentz boost.

Angular distribution↗

Algorithms for coordinate reconstruction in position-sensitive virtual Frisch-grid detectors

Arrays of position-sensitive virtual Frisch-grid (VFG) CdZnTe (CZT) detectors provide a cost-effective solution for integrating large-area arrays for gamma-ray imaging and spectroscopy. These detectors employ high-aspect ratio CZT crystals (bars) with thicknesses up to 50 mm and cross-sections of up to 10 × 10 mm 2 . Despite the long drift distances of charge carriers in such crystals, the detectors have demonstrated excellent performance, achieving energy resolutions better than 1 % full width at half maximum (FWHM) at 662 keV and 3D position resolutions finer than 1 mm. The high spatial resolution is a critical feature of these detectors, as it enables correction of response non-uniformities caused by crystal defects, which remain present even in the highest-quality CZT material. Dislocations and dislocation walls are the primary defects responsible for variations in charge carrier losses as they drift from the interaction points toward the charge-collecting electrodes. The mechanism by which these defects affect carrier transport is generally well understood. Dislocations and sub-grain boundaries act as sinks for carrier-trapping centers, primarily impurities and secondary phases such as tellurium inclusions and precipitates. Here, these regions exhibit significantly higher carrier-trapping rates, leading to variations in the μτ-products. Because the locations of these micron-sized regions are fixed within the detector volume, fluctuations in the total collected charge arise from the random distribution of interaction sites. This results in non-uniform detector responses and degradation of energy resolution. However, by measuring the interaction-site locations with sufficient precision, charge-loss variations can be accurately corrected, allowing recovery of nearly intrinsic energy resolution.

47 OTHER INSTRUMENTATION↗

Beam test performance of AstroPix sensor with 120 GeV protons

AstroPix is a High-Voltage CMOS Monolithic Active Pixel Sensor (HV-CMOS MAPS) developed for precision gamma-ray imaging and spectroscopy in the medium-energy regime, as well as for precise shower imaging and tracking in the Barrel Imaging Calorimeter (BIC) of the Electron Proton/Ion Collider (ePIC) detector at the future Electron–Ion Collider (EIC). We present beam test results of the AstroPix_v3 sensor using a 120 GeV proton beam at the Fermilab Test Beam Facility (FTBF), performed as part of the broader experimental campaign for the BIC prototype calorimeter. The sensor’s 500 µm pixel pitch enabled precise measurement of the beam profile, providing important information for the calorimeter performance studies. Using the measured 120 GeV proton data, we measure the energy deposit of minimum ionizing particles (MIP) and use them to extract the corresponding effective depletion depth at a single bias voltage of −150 V .

AstroPix↗

Investigation of the excited states of 114 Sn using the GRIFFIN spectrometer at TRIUMF

The semi-magic 110-122 Sn isotopes display signs of shape coexistence in their excited 0 + states, which, in contrast to the spherical 0+ ground states, are deformed. Here, this paper investigates the nuclear structure of 114 Sn using the competing β + decay and electron capture of a radioactive beam of 114 Sb produced at the TRIUMF-ISAC facility using the GRIFFIN spectrometer. This study will allow for an in-depth understanding of the excited 0 + states in 114 Sn, by focusing on their decay patterns. In the present experiment, transitions at 856.2-keV and 1405.0-keV, which were observed in an earlier β + decay study but not placed in the 114 Sn level scheme, have been Physics, assigned to the level scheme in connection to the 0$^+_3$ level at 2156.0-keV. Properly assigning these transitions refines the level scheme and enhances our understanding of the nuclear structure in 114 Sn.

GRIFFIN↗

Neutron capture measurements at UMass lowell research reactor

A new facility was designed around the thermal column beam port of the 1 MW Research Reactor at the University of Massachusetts Lowell. Thermal neutrons are collimated to a 1-inch diameter beam and incident on samples to induce the radiative neutron capture. New measurements of capture gamma rays are planned for Mn, Cu, Ni, Cr, and Gd samples in the next few years. The experiments will be carried out in close collaboration with the ENSDF (Evaluated Nuclear Structure Data File) evaluation group at Brookhaven National Laboratory. The gamma rays are measured using an array of high-resolution HPGe detectors. Some of the HPGe detectors use active Compton shields that were designed from scintillation detectors and improve significantly the signal-to-background in the measured gamma-ray spectra with HPGe. The experimental spectra will be validated by the GEANT4 simulations of the array and theoretical models of the emission of gamma rays from the compound nucleus. In conclusion, the new experimental results on the capture gamma ray intensities will be incorporated in future ENSDF evaluations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

59 Co(p,X) spallation reaction cross sections for 250 MeV to 2 GeV protons

Cobalt is an advantageous target for probing the physics of nuclear spallation, because it is a naturally mono-isotopic element ( 59 Co), and its per-nucleon binding energy (BE/A = 8.768 MeV) is near the maximum value for all nuclei. We measured nuclear spallation cross sections for the 59 Co(p,X) reaction at five kinetic energies ranging from 250 MeV to 2 GeV. Cross sections for the production of 58 Co, 57 Co, 57 Mn, 56 Co, 56 Mn, 56 Cr, 55 Fe, 53 Fe, 54 Mn, 52 Mn, 51 Cr, 49 Cr, 48 V, 47 Sc, 46 Sc, 44 Sc, and 44 Scm are reported. Where comparable data exist in the EXFOR reaction database, we find that our measured cross sections generally agree. In many cases, we provide data for reactions or energies not currently reported in EXFOR. Our cross sections also provide evidence for the presence of α-clusters within the 59 Co nucleus, a surprising result given the asymmetry in Z (27) and N (32) for this nucleus. Finally, we use our measurements to evaluate the accuracy of spallation cross section simulations from GEANT4-based radiation transport toolkit, performed with the INCLXX-, Bertini-, and Binary-ion-cascade (BIC) based physics lists. This benchmarking activity revealed that the simulations overestimated the cross sections by a factor of ∼2–4 on average, and that the INCL-XX physics list provides the most reliable results. This evaluation informs the selection of the GEANT4 physics lists used for the analysis of data from NASA’s Psyche mission, which will measure γ rays and neutrons resulting from spallation reactions occurring on the surface of an asteroid whose surface is thought to be rich in iron-nickel metal.

43 PARTICLE ACCELERATORS↗

Generation of radioisotopes for medical applications using high-repetition, high-intensity lasers

We used the PW high-repetition laser facility VEGA-3 at Centro de Láseres Pulsados in Salamanca, with the goal of studying the generation of radioisotopes using laser-driven proton beams. Various types of targets have been irradiated, including in particular several targets containing boron to generate α-particles through the hydrogen–boron fusion reaction. We have successfully identified γ-ray lines from several radioisotopes created by irradiation using laser-generated α-particles or protons including 43 Sc, 44 Sc, 48 Sc, 7 Be, 11 C and 18 F. We show that radioisotope generation can be used as a diagnostic tool to evaluate α-particle generation in laser-driven proton–boron fusion experiments. We also show the production of 11 C radioisotopes, ≈ 6 × 10 6 , and of 44 Sc radioisotopes, ≈ 5 × 10 4 per laser shot. This result can open the way to develop laser-driven radiation sources of radioisotopes for medical applications.

gamma ray spectroscopy↗

Gamma Decay of the 154 Sm Isovector Giant Dipole Resonance: Smekal-Raman Scattering as a Novel Probe of Nuclear Ground-State Deformation

𝛾 decays of the isovector giant dipole resonance (IVGDR) of the deformed nucleus 154 Sm were measured using 2$^{+}_{1}$-Smekal-Raman and elastic scattering of linearly polarized, quasimonochromatic photon beams. The two scattering processes were disentangled through their distinct angular distributions. Their branching ratio and cross sections were determined at six excitation energies covering the 154 Sm IVGDR. Both agree with the predictions of the geometrical model for the IVGDR and confirm 𝛾 decay as an observable sensitive to the structure of the resonance. Consequently, the data place strong constraints on the nuclear shape, including the degree of triaxiality. The derived 154 Sm shape parameters 𝛽 = 0.2925⁢(25) and 𝛾 = 5.0⁢(15)° agree well with other measurements and recent Monte Carlo shell-model calculations.

150 ≤ A ≤ 189↗

Enhanced sensitivity to trace 238 U impurity of sapphire via coincidence neutron activation analysis

Sapphire has mechanical and electrical properties that are advantageous for the construction of internal components of radiation detectors such as time projection chambers and bolometers. However, it has proved difficult to assess its 232 Th and 238 U content down to the picogram per gram level. Here, this work reports an experimental verification of a computational study that demonstrates 𝛾⁢𝛾 coincidence counting, coupled with neutron activation analysis (NAA), can reach ppt sensitivities. Combining results from 𝛾⁢𝛾 coincidence counting with those of earlier single-𝛾 counting based NAA shows that a sample of Saint Gobain sapphire has 232 Th and 238 U concentrations of <0.26 ppt and <2.3 ppt, respectively; the best constraints on the radiopurity of sapphire.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗