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Spectroscopic quadrupole moments in 124 $\mathrm{Xe}$

The Xe isotopic chain with four valence protons above the Z=50 shell closure is an ideal laboratory for the study of the evolution of nuclear deformation. At the N=82 shell closure, 136 Xe presents all characteristics of a doubly closed shell nucleus with a spherical shape. In the very neutron-deficient isotopes close to N=50, the α-decay chain of Xe was investigated to probe the radioactive decay properties near the drip-line and the magicity of 100 Sn. Additionally, the Xe isotopes present higher order symmetries in the nuclear deformation such as the octupole degree of freedom near N=60 and N=90 or O(6) symmetry in stable isotopes. The relevance of the O(6) symmetry has been investigated by measuring the spectroscopic quadrupole moment of the first excited states in 124 Xe. In the O(6) symmetry limit, the spectroscopic quadrupole moment of collective states is expected to be null. A stable 124 Xe beam with energies of 4.03A MeV and 4.11 A MeV was used to bombard a nat W target at the GANIL facility. Excited states were populated via the safe Coulomb excitation reaction. The collision of the heavy ions with a large Z at low energy make this reaction sensitive to the diagonal E2 matrix element of the excited states. The recoils were detected in the VAMOS++ magnetic spectrometer and the γ rays in the AGATA tracking array. The least squares fitting code gosia was used for the analysis to extract both E2 and M1 transitional and E2 diagonal matrix elements. The rotational ground state band was populated up to the 8$^{+}_{1}$ state as well as the 2$^{+}_{2}$ and 4$^{+}_{2}$ states. Using high precision spectroscopic data to constrain the gosia fit, the spectroscopic quadrupole moments of the 2$^{+}_{1}$, 4$^{+}_{1}$, and 6$^{+}_{1}$ states were determined for the first time. The spectroscopic quadrupole moments were found to be negative, large, and constant in the ground state band underlining the prolate axially deformed ground state band of 124 Xe. Here, the present experimental data confirm that the O(6) symmetry is substantially broken in 124 Xe .

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Going to the Bottom of the Explosion that Formed Cas A

The purpose of this INTEGRAL AO 1 proposal was to observe the gamma-ray lines at 1157 keV, as well as 68 keV and 78 keV of the (44)Ti decay chain from the youngest known galactic supernova remnant Cas A. The radioactive decay of (44)Ti in Cas A was first detected by COMPTEL in the 1157 keV line and later confirmed in the lower energy lines using BeppoSAX data. Despite the second confirming measurement, the flux value still has a considerable error, due to a low signal over background ratio and the poor definition of the continuum background in the range of 70 - 100 keV above the line energies. In addition to improving this flux measurement, INTEGRAL has the unique capability, in principle, to measure the line width of the emission. This type of measurement can further constrain supernova explosion models. Unfortunately, the INTEGRAL instrumental background, especially in the SPI spectrometer, turned out to be significantly higher than estimated at the time of proposal submission before launch. This, and to a smaller extent the reduced effective exposure time of about 1.5 Ms compared to requested 2.5 Ms, has precluded us from reaching the sensitivity necessary for this measurement. Studies of the background variability with the goal of improving background modeling are ongoing, and additional 2.5 Ms observing time has just been approved for the next observing cycle.

Oberlack, Uwe↗

New Technique for Barium Daughter Ion Identification in a Liquid Xe-136 Double Beta Decay Experiment

This work addresses long-standing issues of fundamental interest in elementary particle physics. The most important outcome of this work is a new limit on neutrinoless double beta decay. This is an extremely rare and long-sought-after type of radioactive decay. If discovered, it would require changes in the standard model of the elementary constituents of matter, and would prove that neutrinos and antineutrinos are the same, a revolutionary concept in particle physics. Neutrinos are major components of the matter in the universe that are so small and so weakly interacting with other matter that their masses have not yet been discovered. A discovery of neutrinoless double beta decay could help determine the neutrino masses. An important outcome of the work on this project was the Colorado State University role in operating the EXO-200 neutrinoless double beta decay experiment and in analysis of the data from this experiment. One type of double beta decay of the isotope 136 Xe, the two-neutrino variety, was discovered in this work. Although the other type of double beta decay, the neutrinoless variety, was not yet discovered in this work, a world’s best sensitivity of 1.9x10 25 year half-life was obtained. This result rules out a previous claim of a positive result in a different isotope. This work also establishes that the masses of the neutrinos are less than one millionth of that of electrons. A unique EXO-200 analysis, in which the CSU group had a leading role, has established for the first time ever in a liquid noble gas the fraction of daughter atoms from alpha and beta decay that are ionized. This result has important impact on other pending studies, including nucleon decay and barium tagging. Novel additional discoveries include multiphoton ionization of liquid xenon with UV pulsed lasers, which may find application in calibration of future noble liquid detectors, and studies of association and dissociation reactions of Ba + ions in gaseous xenon. Through this project, we are substantially closer to demonstrating “barium tagging”, i.e., detection of single daughter 136 Ba atoms from 136 Xe double beta decay. Milestones achieved include obtaining spectra of small numbers of Ba atoms and cryoprobe advances toward trapping single 136 Ba atoms in solid xenon and probe extraction for detection. One of the other benefits to society is the training of six Ph.D. students in a variety of state-of-the-art technologies, half under primary support of this grant and half with partial support, with four finishing their Ph.D. degrees and two well on their way.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Update to the Performance Assessment for the Savannah River Site Saltstone Disposal Facility - 20124

In 2019, Savannah River Remediation developed a revision to the performance assessment (PA) on behalf of the U.S. Department of Energy (DOE) Savannah River Operations Office (SR) for the near-surface disposal of low-level waste at the Savannah River Site (SRS) Saltstone Disposal Facility (SDF). Soluble waste from SRS Tank Farms undergoes salt processing to remove cesium and other high activity constituents. The low-activity decontaminated salt solution (DSS) is then immobilized by mixing it into a cementitious waste form known as saltstone. After mixing, the saltstone is poured into leak-tight concrete vaults, known as saltstone disposal units (SDUs), where the waste form cures. By the time of facility closure, the SDF is expected to consist of 15 SDUs with a combined capacity of 1.06 E+09 L (280 Mgal) of cured saltstone. The facility operates under a Disposal Authorization Statement (DAS) from DOE and a permit from the South Carolina Department of Health and Environmental Control (SCDHEC). Since the start of operations in 1990, the SDF has received almost 6.7 E+07 L (18 Mgal) of DSS, resulting in the safe disposal of 2.7 E+16 Bq (7.3 E+05 Ci) of activity. Due to the radioactive decay of short-lived contaminants, the total remaining activity in the disposed waste is estimated to be approximately 1.4 E+16 Bq (3.9 E+05 Ci), as of September 2018. The Disposal Authorization Statement requires a demonstration that the system of engineered and natural features of the disposal facility will limit releases from the facility and be protective of human health and the environment for at least the next 1,000 years. The long-term performance of the facility was evaluated under the requirements of the DoE's Radioactive Waste Management Manual (US DOE Manual 435.1-1). Simulations were performed to demonstrate that the disposal facility would meet performance objectives specified in the manual. The evaluation was based on numerical models that simulate the releases of contaminants from the saltstone waste form. Contaminants were transported through groundwater and air pathways to points of assessment to evaluate compliance. In addition, the potential consequences of an inadvertent human intrusion (IHI) were also evaluated. In accordance with the guidance and recommendations in US DoE's technical standard for DAS, deterministic and probabilistic analyses were performed to demonstrate the SDF system, which includes the engineered cover system, the SDUs, the waste form, and the natural features of the site, provides a reasonable expectation that saltstone disposal will meet performance objectives. Post-closure doses to future members of the public (MOP) were evaluated; dose estimates from the air pathway were well below the 1.0 E-04 Sv/yr (10 mrem/yr) performance objective within 1,000 years, and the calculated doses to the MOP from all exposure pathways, including the groundwater and air pathways, were well below the 2.5 E-04 Sv/yr (25 mrem/yr) performance objective within 1,000 years. Doses following an assumed intrusion event within the facility boundaries were well below the IHI performance objectives, where the acute IHI dose was below the acute IHI dose performance objective of 5.0 E-03 Sv (500 mrem) and the chronic IHI dose was below the chronic IHI dose performance objective of 1.0 E-03 Sv/yr (100 mrem/yr) within 1,000 years. (author)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Radioactivity and thermalization in the ejecta of compact object mergers and their impact on kilonova light curves

One promising electromagnetic signature of compact object mergers are kilonovae: approximately isotropic radioactively powered transients that peak days to weeks post-merger. Key uncertainties in kilonova modeling include the emission profiles of the radioactive decay products—non-thermal β-particles, α-particles, fission fragments, and γ-rays—and the efficiency with which their kinetic energy is absorbed by the ejecta. The radioactive energy emitted, along with its thermalization efficiency, sets the luminosity budget and is therefore crucial for predicting kilonova light curves. We outline uncertainties in the radioactivity, describe the processes by which the decay products transfer energy to the ejecta, and calculate time-dependent thermalization efficiencies for each particle type. We determine the net thermalization efficiency and explore its dependence on r-process yields—in particular, the production of α-decaying translead nuclei—and on ejecta mass, velocity, and magnetic fields. We incorporate our results into detailed radiation transport simulations, and calculate updated kilonova light curve predictions. Thermalization effects reduce kilonova luminosities by a factor of roughly 2 at peak, and by an order of magnitude at later times (15 days or more after explosion). We present analytic fits to time-dependent thermalization efficiencies, which can be used to improve light curve models. We revisit the putative kilonova that accompanied gamma-ray burst 130603B, and estimate the mass ejected in that event. We find later time kilonova light curves can be significantly impacted by α-decay from translead isotopes; data at these times may therefore be diagnostic of ejecta abundances.

79 ASTRONOMY AND ASTROPHYSICS↗

Determination of indoor radon concentrations at the elementary schools of Fatih district in Istanbul

Radon is an odorless, tasteless, colorless noble radioactive gas which is produced within the radioactive decay chain of Uranium. The Radon forms in rocks, diffuses into soil and then escapes into atmosphere. When human exposure to high concentration of radon gas from inside, risk of developing lung cancer is increased. There are many methods to determine {sup 222}Rn concentration in the air. In this study, radon concentration of confined air spaces were measured by using LR-115 solid state nuclear track detectors. 509 LR-115 nuclear trace detectors were placed to 25 schools in Fatih District and they effective dose values were calculated. The results of measurements showed that the radon concentration varies between 40-395 Bq/m{sup 3}. This results compared with Turkey’s limits (400 Bq/m{sup 3}) are low, conversely higher compared with WHO’s limits (100 Bq/m{sup 3}).

07 ISOTOPE AND RADIATION SOURCES↗

Molecular Dynamics Simulations of Helium Bubble Formation in Palladium Tritides [Slides]

Pd readily absorbs hydrogen and its isotopes, and can be used to purify gas mixtures involving tritium. Tritium decays to He, forming He bubbles. Bubbles causes possible PCT effects swelling, He release, all leading to failures. Radioactive decay experiments take many years. Molecular dynamics (MD) studies can be quickly done. No previous MD methods can simulate He bubble nucleation and growth.

74 ATOMIC AND MOLECULAR PHYSICS↗

Molecular Dynamics Simulations of Helium Bubble Formation in Palladium Tritides [Slides]

Pd readily absorbs hydrogen and its isotopes, and can be used to purify gas mixtures involving tritium. Tritium decays to He, forming He bubbles. Bubbles causes possible PCT effects swelling, He release, all leading to failures. Radioactive decay experiments take many years. Molecular dynamics (MD) studies can be quickly done. No previous MD methods can simulate He bubble nucleation and growth.

74 ATOMIC AND MOLECULAR PHYSICS↗

Beta decay and the origin of biologial chirality - New experimental results

The hypothetical connection developed by Vester and Ulbricht (1959), between the handedness of beta particles in radioactive decay and the (L) sign of biologial chirality is investigated in a radiolysis experiment. The experiment measured the predicted asymmetry in the formation triplet or 'ortho-' positronium (oPs) in amino acid enantiomers by low energy positrons under conditions of helicity reversal. The positrons were focused on amino acid powder samples. By measuring the time between positron arrival and emission of gamma rays, long-lived oPs were separated from other species. It is found that the asymmetry in leucine (0.8 x 10 to the -4th) is consistent with the theoretical prediction of 10 to the -6th. Neither the experimental limits nor the theoretical estimates are found to rule out a mechanism like that described by Vester and Ulbricht as the cause of the sign of the observed chiral polarization.

Van House, J.↗

Starting DIADEM medium-level waste interim storage's construction - 15034

As part of its decommissioning policy, the nuclear energy division of CEA has identified materials whose high enough radioactive features authorize neither sustainable storage in existing facilities nor evacuation to a French operational geological disposal. Pending availability of definitive solutions, it was decided to explore the possibility to store these materials in a new installation, the subject of DIADEM project [1]. The need was first identified in Marcoule's site, especially to accommodate future waste dismantling of Phenix reactor. Quickly the interest of a centralized storage for all CEA waste of this type appeared to bring together the best expertise to the design and operation of storage. Waste will be stored either to use benefits of radioactive decay or to wait for the commissioning of a new disposal. DIADEM is designed for an operating estimated lifetime of fifty years. This paper deals with the prior safety assessment completed in 2014, the project management and the first steps of the facility construction. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Problems Related to Temperature-Induced Processes in Long-Term Repositories for Nuclear Waste - 17514

Concepts for the final disposal of high level radioactive waste in deep geological formations must consider the heat pulse produced from radioactive decay during operations and in the post-closure phase as an important factor for the integrity of barrier systems. Several safety cases in different countries limit the maximum temperature at the boundary between the technical barrier/canister surface to the host rock/buffer material to 100 C. Increases in maximum temperature have very diverse effects with respect to the type, intensity and range of the heat pulse. These depend, among other factors, on i) the amount of heat emitted, ii) the type of host rock including site-specific characteristics, iii) the safety and repository concept and further site-specific boundary conditions. The German Commission on the Disposal of High-level Radioactive Waste (Commission) recommended, for precautionary reasons, that the temperature limit at the outer surface of waste containers should not exceed 100 C. Higher temperatures could only be considered if the maximum physically possible temperatures in the respective host rock have been reliably set as a result of research findings. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Resolution of a discrepancy in the γ-ray emission probability from the β decay of 137 Ce g

We have deduced the emission probability of the 447-keV γ ray from the ε + β + decay of Ce g 137 (9.0 h) relative to that of the 254-keV γ ray from the Ce m 137 (34.4 h) decay in transient equilibrium. The time-dependent factor in transient equilibrium was applied following the Bateman equation for a radioactive decay chain. The isotope was produced via the La 139 ( p , 3 n ) Ce m , g 137 reaction by bombarding nat La with a proton beam from the 88-in. cyclotron at Lawrence Berkeley National Laboratory. γ -ray intensities were measured using an HPGe detector. The emission probability for the 447-keV γ ray deduced in this work is 1.21(3) (that is 1.21 ± 0.03) per hundred parent decays, which differs significantly from an earlier published value of 2.24(10). We identify the source of this discrepancy to be an incorrect use of the time-dependent factor. Additionally, we have deduced the emission probability of the 504-keV γ ray from the decay of Y g 85 (2.68 h) relative to that of the 232-keV γ ray from the Sr m 85 (1.127 h) decay in transient equilibrium. The isotope was produced via the Sr 86 ( p , 2 n ) Y g 85 reaction by bombarding SrCO 3 86 with a proton beam at the same facility. Overall, the study confirms the assumption of the time-dependent correction for recommending the emission probability of the 504-keV γ ray in the literature. Our work highlights the importance of explicit description by authors of any time-dependent correction they have made when reporting γ -ray intensities for nuclides in transient equilibrium. The need and significance of accurate and precise decay data of Ce g 137 and Y g 85 in basic science and medicine is briefly outlined.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The FRIB Decay Station: New Horizons with Rare Isotopes

In May 2022, the Facility for Rare Isotope Beams (FRIB), located on the campus of Michigan State University (MSU), began delivering exotic isotopes to an international community of scientists. New discoveries are now being reported from radioactive decay of neutron-rich nuclei near N = 20 and N = 28.FRIB is expected to produce roughly 80% of the unstable or radioactive isotopes predicted to exist up to uranium (Z = 92). The new user facility is supported by the U.S. Department of Energy, and it is operated by MSU. A high-power superconducting linear accelerator, shaped like a paper-clip, drives the production of these rare isotopes by colliding stable nuclei moving at half the speed of light with a rotating, water-cooled graphite tar-get. These collisions cause the primary stable beam to fragment into a wide variety of unstable nuclei, which can be subsequently filtered through a multistage magnetic separator, the Advanced Rare Isotope Separator, and transported to one of several experimental stations. The FRIB Decay Station initiator (FDSi) (see Figure 1) was developed to enable comprehensive radio-active decay studies of the exotic nuclei produced by FRIB and it was used in the first two experiments in 2022. Further, the FDSi is a highly reconfigurable multidetector system with two focal planes (FP1 for discrete spectroscopy and FP2 for total absorption spectroscopy) that can be optimized for the specific science goals of each experiment. It is designed, built, and operated by a community of users with the sup-port of U.S. funding agencies, including the Department of Energy and National Science Foundation.

07 ISOTOPE AND RADIATION SOURCES↗

Optical emission from a kilonova following a gravitational-wave-detected neutron-star merger

The merger of two neutron stars has been predicted to produce an optical–infrared transient (lasting a few days) known as a ‘kilonova’, powered by the radioactive decay of neutron-rich species synthesized in the merger. Evidence that short γ-ray bursts also arise from neutron-star mergers has been accumulating. In models of such mergers, a small amount of mass (10 -4 –10 -2 solar masses) with a low electron fraction is ejected at high velocities (0.1–0.3 times light speed) or carried out by winds from an accretion disk formed around the newly merged object. This mass is expected to undergo rapid neutron capture (r-process) nucleosynthesis, leading to the formation of radioactive elements that release energy as they decay, powering an electromagnetic transient. A large uncertainty in the composition of the newly synthesized material leads to various expected colours, durations and luminosities for such transients. Observational evidence for kilonovae has so far been inconclusive because it was based on cases of moderate excess emission detected in the afterglows of γ-ray bursts. Here we report optical to near-infrared observations of a transient coincident with the detection of the gravitational-wave signature of a binary neutron-star merger and with a low-luminosity short-duration γ-ray burst. Our observations, taken roughly every eight hours over a few days following the gravitational-wave trigger, reveal an initial blue excess, with fast optical fading and reddening. Using numerical models, we conclude that our data are broadly consistent with a light curve powered by a few hundredths of a solar mass of low-opacity material corresponding to lanthanide-poor (a fraction of 10 -4.5 by mass) ejecta.

Arcavi, Iair↗

Heavy Element Spectroscopy in the Gas Phase

Actinides are inherently unstable and undergo nuclear decay processes with a concurrent release of energy. Consequently, they are used for nuclear power generation, nuclear weapons, and nuclear medicine. However, the radioactive decay processes also pose significant technological problems for the safe treatment and storage of spent nuclear materials. Cost-effective extraction of the actinides is the key first step in the remediation of nuclear waste, but the appropriate chemical means have yet to be determined. Our present understanding of the chemistry of actinides is limited, with the role of the 5f electrons posing a set of particularly challenging questions. The work reported here is focused on the use of electronic spectroscopy to probe the bonding of small molecules in the gas phase that contains thorium or uranium. Analyses of these data, carried out within the framework of ligand field theory, reveal clear evidence that the 5f electrons are spectators that retain their atomic metal ion character.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Elucidating the Radiation-Induced Redox Chemistry of Plutonium Under Used Nuclear Fuel Reprocessing Conditions

Plutonium plays a critical role in the development of sustainable nuclear fuel cycles, and yet, our fundamental understanding of this element’s inherent radiation-induced redox chemistry and associated impacts on nuclear fuel cycle technologies is limited. Unanticipated changes in oxidation state distribution can influence the speciation and transport of plutonium in a given process. Control of these parameters is especially important for used nuclear fuel reprocessing technologies, wherein the separation and recovery of plutonium is typically achieved by the selective formation, maintenance, and complexation of specific oxidation states. Furthermore, plutonium’s inherent radiation-induced redox chemistry has the capacity to influence the radiolytic behavior of its complexes, the longevity of which are critical in the design of efficient and cost-effective advanced reprocessing technologies. These radiation-induced processes are unavoidable under fuel cycle conditions owing to the inherency of ionizing radiation fields to the decay of plutonium’s isotopes and to the various other radioisotopes generated by nuclear fission and neutron-capture process and the subsequent radioactive decay of their products. As such, mechanistically understanding the response of plutonium’s multiple oxidation states to multi-component ionizing radiation fields is essential for predicting the behavior of this critical element under used nuclear fuel reprocessing conditions. Here, through a combination of time-resolved (electron pulse) and steady-state (alpha and gamma) irradiation experiments complemented by quantitative, multiscale modeling calculations, we present advances in our understanding of radiation-induced plutonium redox chemistry!

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Proof of principle study: synchrotron X-ray fluorescence microscopy for identification of previously radioactive microparticles and elemental mapping of FFPE tissues

Biobanks containing formalin-fixed, paraffin-embedded (FFPE) tissues from animals and human atomic-bomb survivors exposed to radioactive particulates remain a vital resource for understanding the molecular effects of radiation exposure. These samples are often decades old and prepared using harsh fixation processes which limit sample imaging options. Optical imaging of hematoxylin and eosin (H&E) stained tissues may be the only feasible processing option, however, H&E images provide no information about radioactive microparticles or radioactive history. Synchrotron X-ray fluorescence microscopy (XFM) is a robust, non-destructive, semi-quantitative technique for elemental mapping and identifying candidate chemical element biomarkers in FFPE tissues. Still, XFM has never been used to uncover distribution of formerly radioactive micro-particulates in FFPE canine specimens collected more than 30 years ago. In this work, we demonstrate the first use of low-, medium-, and high-resolution XFM to generate 2D elemental maps of ~ 35-year-old, canine FFPE lung and lymph node specimens stored in the Northwestern University Radiobiology Archive documenting distribution of formerly radioactive micro-particulates. Additionally, we use XFM to identify individual microparticles and detect daughter products of radioactive decay. The results of this proof-of-principle study support the use of XFM to map chemical element composition in historic FFPE specimens and conduct radioactive micro-particulate forensics.

62 RADIOLOGY AND NUCLEAR MEDICINE↗