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Novel methods for TH-229 production through fast neutron irradiation of TH-23F0 and charged particle irradiation of Th-230 and Th-232. Final Report DE-SC0020140

The activities and results of research related to accelerator production of Pa and Th isotopes via bombardment of 230 Th and 232 Th targets are described herein. This research was supported through DOE grant DE-SC0020140 and was conducted in collaboration with Oak Ridge National Laboratory and Lawrence Berkeley National Laboratory. Cross section measurements, transport model and nuclear physics model calculations are presented. Highlights include the first ever measurements of 229 Pa, two publications, and graduation of a PhD student.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Raman signatures from age-dating PuO 2 since last calcination

The self-irradiation of PuO 2 has been shown to affect the attributes of fifteen vibrational bands in the Raman spectrum. The vibrational bands correspond to the Raman allowed vibrational mode T 2g , overtones, defects, and bands from electronic origin. Defects in the crystal lattice from low-calcination temperature and alpha decay origins are responsible for the changes in the band attributes (band position, full-width half maximum (FWHM), intensity). Crystal lattice defects are also responsible for the growth of the defect bands. The temporal behavior of the vibrational bands can be used to estimate the age of the material since last calcination. Laser annealing was used to reset the material to full crystallinity prior to the aging study. 240 PuO 2 , with an alpha decay rate of 3.67 greater than the decay rate of 239 PuO 2 , was primarily used to assess the alpha decay-induced damage within 3 years. The aging study focused on the time-dependent properties of the T 2g band and the growth of defect bands. The FWHM of the T 2g band and the ratio of the areas of the defect bands/T 2g band were measured through a time period in excess of 3 years. The data from this study were found very close to the data describing the temporal evolution of the lattice constant measured with the X-ray diffraction (XRD) technique. The local physical properties of the material measured with Raman spectroscopy and the lattice parameter constant measured with XRD indicates a strong correlation between the two techniques. Although both techniques provide similar age-dating information, in contrast to the few milligram quantities required for XRD, Raman spectroscopy requires a 10 µm diameter PuO 2 particle to provide an estimate of the material age since last calcination.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Defect characterization and charge transport measurements in high-resolution Ni/n-4H-SiC Schottky barrier radiation detectors fabricated on 250 μ m epitaxial layers

Advances in the growth processes of 4H-SiC epitaxial layers have led to the continued expansion of epilayer thickness, allowing for the detection of more penetrative radioactive particles. In this work, we report the fabrication and characterization of high-resolution Schottky barrier radiation detectors on 250 μm thick n-type 4H-SiC epitaxial layers, the highest reported thickness to date. Several 8 × 8 mm 2 detectors were fabricated from a diced 100 mm diameter 4H-SiC epitaxial wafer grown on a conductive 4H-SiC substrate with a mean micropipe density of 0.11 cm -2 From the Mott–Schottky plots, the effective doping concentration was found to be in the range (0.95–1.85) × 10 14 cm -3 , implying that full depletion could be achieved at ~5.7 kV (0.5 MV/cm at the interface). The current-voltage characteristics demonstrated consistently low leakage current densities of 1–3 nA/cm 2 at a reverse bias of -800 V. This resulted in the pulse-height spectra generated using a 241Am alpha source (5486 keV) manifesting an energy resolution of less than 0.5% full width at half maximum (FWHM) for all the detectors at -200 V. The charge collection efficiencies (CCEs) were measured to be 98–99% with no discernable correlation to the energy resolution. A drift-diffusion model fit to the variation of CCE as a function of bias voltage, revealed a minority carrier diffusion length of ~10 μm. Deep level transient spectroscopy measurements on the best resolution detector revealed that the excellent performance was the result of having ultralow concentrations of the order of 1011 cm-3 lifetime limiting defects—Z 1/2 and EH 6/7 .

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Revisiting GeV-scale annihilating dark matter with the AMS-02 positron fraction

Antimatter cosmic-rays are used to probe new phenomena in physics, including dark matter annihilation. Here, we use the cosmic-ray positron fraction spectrum by the Alpha Magnetic Spectrometer, to search for such an annihilation signal in the Galaxy. We focus on dark matter with mass between 5 and 120 GeV, producing high-energy electrons and positrons. In these cosmic-ray energies the interplay of multiple astrophysical sources and phenomena, makes this search highly sensitive to the underlying astrophysical background assumptions. We use a vast public library of astrophysical models for the cosmic-ray positron fraction background, to derive robust upper limits on the dark matter's annihilation cross section for a number of annihilation channels. This library accounts for different types of cosmic-ray sources and uncertainties on their distribution in space and time. Also, it accounts for uncertainties on those sources' output, their injected into the interstellar medium cosmic-ray spectra and for uncertainties on cosmic-ray propagation. For any given dark matter particle mass and annihilation channel, upper limits on the annihilation cross section are given by bands that stretch a full order of magnitude in its value. Our work provides weaker limits compared to earlier results, that are however robust to all the relevant astrophysical uncertainties. Between 5 and 15 GeV, we find indications for a possible excess flux of cosmic-ray electrons and positrons. That excess is found for most, but not all of our astrophysical background parameter space, and its significance can vary appreciably. Further scrutiny is necessary to improve the understanding of these lower energy cosmic rays. Finally, we note that even if an excess signal is found in these energies, the current background uncertainties do not allow us to accurately deduce its underlying particle properties.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Calibration sources for the LEGEND-200 experiment

In the search for a monochromatic peak as the signature of neutrinoless double beta decay an excellent energy resolution and an ultra-low background around the Q-value of the decay are essential. The LEGEND-200 experiment performs such a search with high-purity germanium detectors enriched in 76 Ge immersed in liquid argon. To determine and monitor the stability of the energy scale and resolution of the germanium diodes, custom-made, low-neutron emission 228 Th sources are regularly deployed in the vicinity of the crystals. Here we describe the production process of the 17 sources available for installation in the experiment, the measurements of their alpha- and gamma- activities, as well as the determination of the neutron emission rates with a low-background LiI(Eu) detector operated deep underground. With a flux of ( 4.27 ± 0.60 stat ± 0.92 syst ) × 10 -4 n / (kBq·s), approximately one order of magnitude below that of commercial sources, the neutron-induced background rate, mainly from the activation of 76 Ge, is negligible compared to other background sources in LEGEND-200.

47 OTHER INSTRUMENTATION↗

The diphoton $$q_T$$ spectrum at N$$^3$$LL$$^\prime $$ + NNLO

Abstract We present a $$q_T$$ q T -resummed calculation of diphoton production at order N $$^3$$ 3 LL $$^\prime $$ ′ + NNLO. To reach the primed level of accuracy we have implemented the recently published three-loop $${\mathcal {O}}(\alpha _s^3)$$ O ( α s 3 ) virtual corrections in the $$q\bar{q}$$ q q ¯ channel and the three-loop transverse momentum dependent beam functions and combined them with the existing infrastructure of , a code performing resummation at order N $${}^3$$ 3 LL. While the primed predictions are parametrically not more accurate, one typically observes from lower orders and other processes that they are the dominant effect of the next order. We include in both the $$q\bar{q}$$ q q ¯ and loop-induced gg channel the hard contributions consistently together at order $$\alpha _s^3$$ α s 3 and find that the resummed $$q\bar{q}$$ q q ¯ channel without matching stabilizes indeed. Due to large matching corrections and large contributions and uncertainties from the gg channel, the overall improvements are small though. We furthermore study the effect of hybrid-cone photon isolation and hard-scale choice on our fully matched results to describe the ATLAS $$\text {8}$$ 8 TeV data and find that the hybrid-cone isolation worsens agreement at small $$q_T$$ q T compared to smooth-cone isolation.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Background identification in cryogenic calorimeters through $\alpha -\alpha$ delayed coincidences

Localization and modeling of radioactive contaminations is a challenge that ultra-low background experiments are constantly facing. These are fundamental steps both to extract scientific results and to further reduce the background of the detectors. Here we present an innovative technique based on the analysis of $\alpha -\alpha$ delayed coincidences in 232 Th and 238 U decay chains, developed to investigate the contaminations of the ZnSe crystals in the CUPID-0 experiment. This method allows to disentangle surface and bulk contaminations of the detectors relying on the different probability to tag delayed coincidences as function of the $\alpha$ decay position.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Alpha/beta-gated gamma–gamma spectroscopy of mixed fission products for trace analysis

This experiment demonstrated that some hard-to-detect fission products can be quantified directly from mixed fission product samples using advanced radio-emission spectroscopy techniques. A gamma/gamma coincidence detector was combined with a custom liquid scintillation counter to evaluate the benefits of alpha and beta coincident and anti-coincident analysis of mixed fission product samples. Reduction factors in the minimum detectable activity (MDA) relative to traditional gamma counting were quantified for a set of radionuclides. For isotopes like 91Y, 144Ce, 147Nd, and 153Sm MDA reductions of factors of 1-2 were observed using optimized beta thresholds. Using beta anti-coincidence counting reductions of factors 3-5 were observed for isotopes like 89Sr, 95mNb, 115Cd, and 137Cs and factors of 5-7 for isotopes like 235U using alpha coincidence counting. The selectivity of gamma/gamma coincidence and reduction in backgrounds using beta gating were also demonstrated with 136Cs and 153Sm. The improvements observed in the detection sensitivity of fission products and actinides achieved by combining time-correlated radiation signatures is significant and of value to applications such as nuclear fission physics, environmental monitoring for nuclear waste, reactor accidental releases, and nuclear forensics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Cluster structure of light nuclei

We review recent studies of the cluster structure of light nuclei within the framework of the algebraic cluster model (ACM) for nuclei composed of k α-particles and within the framework of the cluster shell model (CSM) for nuclei composed of k α-particles plus x additional nucleons. The calculations, based on symmetry considerations and thus for the most part given in analytic form, are compared with experiments in light cluster nuclei. The comparison shows evidence for Z 2 , D 3h and T d symmetry in the even–even nuclei 8 Be (k = 2), 12 C (k = 3) and 16 O (k = 4), respectively, and for the associated double groups Z' 2 and D' 3h in the odd nuclei 9 Be, 9 B (k = 2, x = 1) and 13 C (k = 3, x = 1), respectively.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Data for Spallation Neutron Radioisotope Production (Final Technical Report)

Over 50 million nuclear medicine procedures are performed annually, leading to a multi-billion dollar market for radioisotope production. The demand for new medical and research isotopes is growing, and radioisotope supply is insufficient. Most radioisotope production today utilizes charged particle or low-energy neutron irradiation of a target. Isotope production with tens to hundred MeV incident energies is a relatively unexplored option. There is a tremendous opportunity associated with a growing number of suitable domestic and international facilities buttressed by hundred million dollar global investments (e.g., the Los Alamos and Brookhaven Isotope Production Facilities, the European Spallation Source in Lund, and the Korean Multi-purpose Accelerator Complex in Gyeongbuk). In part due to a lack of supporting nuclear data that would make modeling radioisotope yields and purities possible, these facilities do not utilize their high-energy neutron fluxes for isotope production. This project attempted to measure neutron reaction excitation functions relevant to the large-scale production of critical radioisotopes, enabling development of cost-efficient isotope production methods, contributing to the improvement of theoretical models, and enhancing the value of national isotope production facilities. Reactions which form 67 Cu, 32 Si, and alpha-emitting isotopes like 225 Ac were chosen for their consistent prioritization by expert panels, representation of diverse reaction mechanisms, and relative lack of supporting nuclear data. Accurate measurement of these data is presently made only using quasi-monoenergetic neutron beams, which are produced by bombarding thin lithium targets with protons at only a few laboratories in the world. Ultimately, the projects efforts were incompletely accomplished due to a combination of multi-year technical issues at the only laboratory in the world which can make the proposed measurements, iThemba Labs in South Africa, and the onset of a global pandemic, which precluded the significant effort and time required to develop an independent measurement capability in the United States.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Large Volume Airborne Contamination Monitoring To Support Nuclear Processes' Deactivation and Decommissioning

Current D and D operations at Hanford have demonstrated a flaw in the current state of the art capability of defining airborne contamination boundaries - Airborne particulate emissions of Pu-239 from CM2H operations on the Hanford Pu Finishing Plant were detected well beyond areas controlled for airborne Pu, putting numerous workers at risk for radiological assimilations - Current air samplers and CAM systems were surveying insufficient volumes of air to accurately predict where respiratory protection was required - Hanford is located in a high radon environment, making air monitoring for alpha emitting actinides challenging in high alpha radon induced backgrounds. - Inexpensive HEPA based home and industrial air purifiers filter significantly higher volumes of air than commercially available continuous-air monitoring (CAM) systems. - Inexpensive models capable of filtered air volumes exceeding 1000 times that of a CAM. - Detector system can be built to detect x-rays generated from actinide decay. - Branching ratios of x-rays are 4 orders of magnitude more intense from Plutonium decay than its gamma emissions. - Detector system can be a low resolution systems, as x-ray region of interest is not terribly congested. - Detection systems evaluated will be designed based on slabs of NaI or pixelated NaI or CsI panels. - Simple graphical user interface software will be developed to operate the detection system. - Concept is to deploy some of these air-purifying systems in nonradiological areas around SRNL to confirm radon can be rejected with confidence. - Generate some filters contaminated with plutonium via electroplated Pu or lab generated simulated particles. - then deploy units in known airborne radiological environments to establish systems ability to accurately measure actinide based hot particles Lab analyses will follow up the system analyses to ensure hot particles were correctly identified. Analysis by Scintillation: - Application of scintillation media to the surface of the filters is being explored. - Evaluating slabs of ZnS(Ag), application of powdered ZnS(Cu) and spray on Perkin Elmer Enhance. - Scintillation events would then be digitized with a digital camera and quantified. - Comparing against sensitivity of a PMT or SiPD readout. - Currently evaluating a Thorlabs 8 Megapixel Monochrome Scientific CCD Camera, hermetically sealed cooled package with a wide angle lens. - Wide angle lens allows complete view of HEPA filter from 7 inches away. - Images taken of glow in the dark paint, as well as plutonium-induced fluorescence. - Plutonium was flamed mounted on a 1 inch diameter stainless steel planchet, covered with a layer of mylar and a section of scintillating ZnS obtained from Eljon. - Currently working on reducing signal-to-noise levels to boost sensitivity. - Dark box to hold contaminated or electroplated source covered filters under fabrication. Analysis by x-ray Spectroscopy: - Branching ratios for x-ray emissions from Plutonium isotopes are orders of magnitude more intense than gamma-ray emissions. - The nuclear databases are incomplete on the branching ratios of some of the isotopes. - Evaluating some custom built SrI2 x-ray spectrometers vs a conventional windowed NaI detector. - SrI2 detectors are carbon-composite-windowed 51 mm x 51 mm. - MCNP calculations to establish self absorbance of filter media on 17 keV x-ray. Radon Rejection: - Activated charcoal pre-filter acts as a Radon trap. - Adding a time lapse feature to camera to aid in radon rejection. SRS Plutonium Fuel Form D and D Operations: Currently deploying air sampler to D and D operation of Pu-238 facility at SRS to generate some field samples to analyze.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Discovery of the new isotope 251 Lr and the α-decay fine structure in 253 L

The products of the 203, 205 Tl ( 50 Ti, 2n) fusion-evaporation reactions were studied using the recently commissioned Argonne Gas-Filled Analyzer at Argonne National Laboratory. Two α-decay activities with energies of 9210(19) and 9246(19) keV and half-lives of $42^{+42}_{-14}$ and $24.4^{+7.0}_{-4.5}$ ms were observed which were followed by the known α decays of 247 Md and 243 Es . They are interpreted as originating from the 1/2 ⁻ [521] and 7/2 ⁻ [514] single-proton Nilsson states in the hitherto unknown isotope 251 Lr . From the measured Q α values the 1/2 ⁻ level was placed 117(27) keV above the 7/2 - level in 251 Lr in contrast to 255 Lr where the 1/2 ⁻ level is the lowest. Also, the α decay of 253 Lr was studied in more detail and a new α line at 8660(20) keV was found and a new half-life value of 2.46(32) s for an isomeric state in 253 Lr was measured. The 251, 253, 255 Lr Q α values were compared with predictions of various mass models. The relative energies of the 1/2 ⁻ [521] and 7/2 ⁻ [514] single-proton Nilsson states in 251, 253, 255 Lr isotopes were compared with results of the cranking shell model with pairing treated using the particle-number-conserving method. The level separation and, in particular, the level order change between 251 Lr and 255 Lr was reproduced only when the hexacontetrapole deformation ϵ 6 was included in the calculations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Potassium-Containing α-MnO 2 Nanotubes: The Impact of Hollow Regions on Electrochemistry

α-MnO 2 type materials have been studied as electrode materials in rechargeable batteries and electrocatalysts due to their 2 × 2 tunneled crystal structures capable of accommodating cations and their tunable physiochemical properties. In this study, we deliberately synthesized K + containing α-MnO 2 (K 0.9 Mn 8 O 16 ) hollow nanotubes varying the dimensions of the hollow regions and level of surface defects. The K 0.9 Mn 8 O 16 nanotube material samples have similar crystallinity, thermal stability, and average Mn oxidation state. Oxygen surface defects in the hollow regions were revealed through detailed studies using electron energy loss spectroscopy. The impact of the hollow regions and associated surface defects on the electrochemistry of K x Mn 8 O 16 were investigated using cyclic voltammetry, galvanostatic intermittent titration technique, and galvanostatic cycling. The K 0.9 Mn 8 O 16 nanotubes with a large hollow region (~30 nm) and higher level of surface defects show higher apparent lithium ion diffusion coefficients and lower polarization compared to the nanotubes with a small hollow region (~10 nm). In-situ lithiation demonstrated that the dimensions of the nanotube walls expanded, but the hollow region did not change in size as result of lithiation. Furthermore, this research demonstrates that tuning particle architecture and surface defects can positively impact functional behavior of electrochemical storage materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Rapid recovery of At-211 by extraction chromatography

The near quantitative separation, purification, and recovery of 211 At has been demonstrated through an extraction chromatography process which utilizes porous beads impregnated with 3-octanone, resulting in an elution yield of 92–95%. Moreover, the rapid nature of this process, <20 min, was achieved after dissolution of a Bi metal target in HNO 3 following retrieval from the beamline after α-particle bombardment. The solution was directly loaded onto the column with no volume or acidity adjustment. The column was washed with HNO 3 and H 2 O, and 211 At was eluted with ethanol, collecting roughly 87–93% in 1 mL. This process of recovering high purity 211 At, in near quantitative yields, represents a significant advance in At separations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Gravitational wave detection with plasma haloscopes

Searches for high frequency gravitational waves using cavities based on the Gertsenshtein effect were recently proposed, building off existing axion dark matter experiments. In particular, the sensitivity of axion dark matter experiments using metamaterial plasmas (tunable plasma haloscopes) to gravitational waves has not been explored in detail. Here we perform a full analysis of gravitational wave detection in plasma haloscopes, showing that the baseline design of experiments such as ALPHA is several orders of magnitude less sensitive than previously thought. We show how simple changes to the experiment can recover that sensitivity and lead to a powerful gravitational wave detector in the 𝒪⁡(10–50) GHz frequency range.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Experimental evidence for low-lying quadrupole isovector excitation of 208 Po

In this study, we present the results from an experiment dedicated to measure the lifetime of the \(2^+_2\) state, candidate for the one-phonon mixed-symmetry state, of \(^{208}\) Po. This nucleus was studied in the \(\alpha \) -transfer reaction \(^{204}\) Pb( \(^{12}\) C, \(^{8}\) Be) \(^{208}\) Po and the lifetime of the \(2^+_2\) state was determined by utilizing the Doppler-shift attenuation method. The experimental data show that the \(2^+_2\) state decays with a sizable M 1 transition to the \(2^+_1\) state revealing its isovector nature.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Subleading power resummation of rapidity logarithms: the energy-energy correlator in $ \mathcal{N} $ = 4 SYM

We derive and solve renormalization group equations that allow for the resummation of subleading power rapidity logarithms. Our equations involve operator mixing into a new class of operators, which we term the “rapidity identity operators”, that will generically appear at subleading power in problems involving both rapidity and virtuality scales. To illustrate our formalism, we analytically solve these equations to resum the power suppressed logarithms appearing in the back-to-back (double light cone) limit of the Energy-Energy Correlator (EEC) in \( \mathcal{N} \) = 4 super-Yang-Mills. These logarithms can also be extracted to \( \mathcal{O}\left({\alpha}_s^3\right) \) from a recent perturbative calculation, and we find perfect agreement to this order. Instead of the standard Sudakov exponential, our resummed result for the subleading power logarithms is expressed in terms of Dawson’s integral, with an argument related to the cusp anomalous dimension. We call this functional form “Dawson’s Sudakov”. Our formalism is widely applicable for the resummation of subleading power rapidity logarithms in other more phenomenologically relevant observables, such as the EEC in QCD, the p T spectrum for color singlet boson production at hadron colliders, and the resummation of power suppressed logarithms in the Regge limit.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Strong coupling in (2+1+1)-flavor QCD

The strong coupling $\alpha_\mathrm{s}$ can be obtained from the static energy as shown in previous lattices studies. For short distances, the static energy can be calculated both on the lattice with the use of Wilson line correlators, and with the perturbation theory up to three loop accuracy with leading ultrasoft log resummation. Comparing the perturbative expression and lattice data allows for precise determination of $\alpha_\mathrm{s}(m_Z)$. We will present preliminary results for the determination of $\alpha_\mathrm{s} {(M_Z)}$ in (2+1+1)-flavor QCD using the configurations made available by the MILC-collaboration with smallest lattice spacing reaching 0.0321~fm.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗