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Evidence for ground-state electron capture of K 40

Potassium-40 is a widespread, naturally occurring isotope whose radioactivity impacts estimated geological ages spanning billions of years, nuclear structure theory, and subatomic rare-event searches—including those for dark matter and neutrinoless double-beta decay. The decays of this long-lived isotope must be precisely known for its use as a geochronometer, and to account for its presence in low-background experiments. There are several known decay modes for potassium-40, but a predicted electron-capture decay directly to the ground state of argon-40 has never been observed. The existence of this decay mode impacts several fields, while theoretical predictions span an order of magnitude. Here we report on the first, successful observation of this rare decay mode, obtained by the KDK (potassium decay) Collaboration using a novel combination of a low-threshold x-ray detector surrounded by a tonne-scale, high-efficiency γ -ray tagger at Oak Ridge National Laboratory. A blinded analysis reveals a distinctly nonzero ratio of intensities of ground-state electron-captures ( I EC 0 ) over excited-state ones ( I EC * ) of I EC 0 / I EC * = 0.0095 ± stat 0.0022 ± sys 0.0010 (68% CL), with the null hypothesis rejected at 4 σ [Stukel et al. , Phys. Rev. Lett. 131 , 052503 (2023) ]. In terms of branching ratio, this unambiguous signal yields I EC 0 = 0.098 % ± stat 0.023 % ± sys 0.010 % , roughly half of the commonly used prediction. This first observation of a third-forbidden unique electron capture improves our understanding of low-energy backgrounds in dark-matter searches and has implications for nuclear-structure calculations. For example, a shell-model based theoretical estimate for the neutrinoless double-beta decay half-life of calcium-48 is increased by a factor of 7 - 2 + 3 . Our nonzero measurement shifts geochronological ages by up to a percent; implications are illustrated for Earth and solar system chronologies.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Data Summary Report for Soil and Slab Sampling at Former Building 175

Lawrence Livermore National Security (LLNS) and the U.S. Department of Energy (DOE) are in the process of returning the area where Building 175 existed to beneficial use for future site development. The completed assessment will help LLNS and DOE to outline project scope and costs associated with the removal, characterization, and disposal of materials generated when the concrete slab for the former building and any associated remaining subsurface structures are demolished. Slab removal under the Transition & Disposition process requires full screening for potential site contamination to determine appropriate future land use. Borehole locations and depths were designed to correctly assess DOE’s future liability for characterizing residual vadose zone contamination. If a residual source area is identified at depth, DOE will need to evaluate the additional cost of future subsurface cleanup (with limited access) due to planned development. This is necessary to leave the location in a “ready-to-build” status. As a result, Phase II sampling requirements may in some cases extend beyond the construction zone required for slab removal to ensure the necessary due diligence. To avoid the potential spread of contamination and/or the creation of an environmental release by impacting the integrity of known contamination areas (e.g., pit within room 102 and the east to west boundary seam), these locations were not sampled for this project. During demolition of the slab, these locations and their underlying soils should be further evaluated. The assessment was conducted in accord with the May 2022 Lawrence Livermore National Laboratory Former Building 175 Assessment Soil Sampling and Analysis Plan / Quality Assurance Plan. Thirty-six, direct-push borings were advanced, along with collecting concrete (where present) and soil samples for laboratory analyses. Thirty-two of the borings were advanced to a depth of 25 feet below ground (bgs), and four borings were advanced to a depth of 55 feet bgs. The concrete slab for former Building 175 ranged from approximately 8 inches to over two feet in thickness. Soils encountered during the investigation consisted primarily of clayey silt, with interbeds of sandy gravel and silty sand to the total depth explored of 55 feet bgs. Field photoionization detector readings – checking for volatile organic compound (VOC) vapors in soils, ranged from zero (0) to a peak of 33 parts per million at 25 feet bgs in boring PC-B175- 028. The cause for the peak reading is unknown, however, no visually discolored or odorous soils were encountered during the assessment and all VOC results were below Lawrence Livermore National Laboratory’s (LLNL’s) Soil Screening and Management Plan (SSMP) soil screening levels (SSL). Groundwater was not encountered during the assessment and is expected to occur at roughly 65 feet bgs in the project area. No metals were detected at concentrations of concern in the concrete core samples collected and analyzed. Low gross alpha and beta activity concentrations were detected in the concrete core samples collected and analyzed. The detected activity concentrations would appear to be from naturally occurring radioactive isotopes, i.e., potassium 40, present in the raw materials used to make concrete and not artificially added. Tritium was not detected above the testing laboratory's Method Detection Limit (MDL) in any of the concrete core samples collected and analyzed. The radioactive isotopes - actinium 228, bismuth 214, lead 212, lead 214, potassium 40, radium 226, radium 228, and thallium 208, were detected at low activity concentrations in the concrete core samples analyzed. Based on the detected activity concentrations, the isotopes would appear to be naturally occurring in the raw materials used to make concrete and not artificially added. Acetone – a common laboratory contaminant, was detected in nine of the soil samples collected and analyzed. Concentrations of two other volatile organic compounds (benzene and tetrachloroethene) were detected in five of the soil samples analyzed. All concentrations were below SSLs. Total petroleum hydrocarbons as diesel range organics were detected at 43.9 milligrams per kilogram (mg/kg) in the 20-foot bgs duplicate sample from boring PC-B175-007. Total petroleum hydrocarbons as motor oil were detected at 7.20 mg/kg in the 15-foot bgs routine sample from boring PC-B175-001, and at 20.7 mg/kg in the 20-foot bgs duplicate sample from boring PC-B175-007. The SSL for diesel-range TPHs is 260 mg/kg. LLNL does not have an SSL for motor oil range TPHs. No indications of a release, e.g., visibly stained, or odorous soil, were present at the boring locations. No samples collected contained polychlorinated biphenyls (PCBs) in concentrations above the laboratory reporting limit. Arsenic was detected above its SSL of 8.51 mg/kg in the 25-foot bgs routine sample collected from boring PC-B175-023. Nickel was detected above its SSL of 86.0 mg/kg in the 10-foot bgs routine sample from boing PC-B175-005, the 20-foot bgs routine sample from boring PC-B175-025, and the 25-foot bgs routine sample from boring PC-B175-034. The detected concentrations, however, were well below ten times (10x) their respective STLCs. Gross alpha and/or gross beta were detected above their respective SSL activity concentrations in three routine soil samples. Retesting (two per sample) of the samples showed that the initial reported activity concentrations were anomalous. Tritium was not detected in any of the routine or duplicate soil samples collected and analyzed during the investigation. The radioactive isotopes - actinium 228, bismuth 212 and 214, lead 212 and 214, potassium 40, radium 224, 226 and 228, thallium 208, thorium 234 and uranium, were detected at low activity concentrations in the soil samples analyzed for radioactive constituents. The detected isotopes and their associated activity concentrations are typical of those naturally occurring in the marine-type sedimentary deposits underlying the Livermore Valley. No radiological controls are necessary for the soil evaluated.

54 ENVIRONMENTAL SCIENCES↗

Nuclear Data Sheets for A=40

The experimental nuclear structure data and decay data are evaluated for the known nuclides of mass 40 (Mg, Al, Si, P, S, Cl, Ar, K, Ca, Sc, Ti). Detailed evaluated nuclear structure information is presented with the best values recommended for level energies, half-lives, γ-ray energies and intensities, decay properties (energies, intensities and placement of radiations), and other spectroscopic data. The {sup 40}Ca and {sup 40}K nuclides remain as the most extensively studied from many different reactions and decays; no excited states are known in {sup 40}Mg, {sup 40}Al, {sup 40}P and {sup 40}Ti. This work supersedes the earlier full evaluation of A=40 by J. Cameron and B. Singh (2004Ca38).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

A novel experimental system for the KDK measurement of the 40 K decay scheme relevant for rare event searches

Potassium-40 ( 40 K) is a long-lived, naturally occurring radioactive isotope. The decay products are prominent backgrounds for many rare event searches, including those involving NaI-based scintillators. 40 K also plays a role in geochronological dating techniques. The branching ratio of the electron capture directly to the ground state of argon-40 has never been measured, which can cause difficulty in interpretingcertain results or can lead to lack of precision depending on the field and analysis technique. Additionally, the KDK (Potassium (K) Decay (DK)) collaboration is measuring this decay. A composite method has a silicon drift detector with an enriched, thermally deposited 40 K source inside the Modular Total Absorption Spectrometer. This setup has been characterized in terms of energy calibration, gamma tagging efficiency, live time and false negatives and positives. A complementary, homogeneous, method is also discussed; it employs a KSr 2 I 5 :Eu scintillator as source and detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

High Resolution Study of 40 Ca to Constrain Potassium Nucleosynthesis in NGC 2419

The globular cluster NGC 2419 was the first to exhibit a Mg-K anticorrelation, linked to hydrogen burning at temperatures between 80-260 MK. However, the key K-destroying reaction, 39 K(p,γ) 40 Ca, has a large rate uncertainty in this range. We significantly constrain this rate with a high resolution 39 K( 3 He,d) 40 Ca study. We resolve the $E$$^{c.m.}_{r}$ = 154 keV resonance in 39 K+p for the first time, increasing the previous rate by up to a factor 13 and reducing its 1σ width by up to a factor of 42. As a result, reaction network calculations for NGC 2419 suggest that this could lower temperatures needed to reproduce the Mg-K anticorrelation.

39 ≤ A ≤ 58↗

A chemical-recovery-free ammonium sulfite-based alkali pretreatment of corn stover for low-cost sugar production via fertilizer use of waste liquor

The production of cellulosic sugars is a pivotal strategy for advancing biomass bioconversion. This study evaluated the pretreatment of corn stover using ammonium sulfite and potassium hydroxide to develop comprehensive data on sugar, lignin, chemicals, and overall mass recovery profiles in a batch reactor at 80 °C. The results indicated significant improvements in delignification, deacetylation, enzymatic digestibility, and overall sugar yield. Specifically, pretreating corn stover with a solution of 40 wt% potassium hydroxide and 15 wt% ammonium sulfite at 80 °C for 2 h achieved 78.9 % lignin removal and 82.1 % acetyl removal, resulting in a total sugar yield exceeding 87.5 % with an enzyme loading of 12.5 mg protein/g-glucan plus xylan. The pretreated spent liquor, containing ammonium, potassium, sulfur, biomass-derived organics, and inorganics, demonstrated substantial potential as a fertilizer. The techno-economic analysis projected a minimum sugar selling price of $0.285 per pound, supporting the ongoing development and implementation of chemical-recovery-free pretreatment technology.

09 BIOMASS FUELS↗

Lowering the Lasing Threshold by Doping in Mid-Infrared Lasers Based on HgCdTe with HgTe Quantum Wells

The possibility of significant lowering of the interband lasing threshold in laser structures of the mid-infrared region based on HgCdTe with HgTe quantum wells by doping with donors, which introduce δ layers near quantum wells, is proposed and analyzed. It is shown that at an optimum surface donor concentration in the δ layer of 4 × 10{sup 10} cm{sup –2} and an operating temperature of >40 K, the lasing threshold at a wavelength of 20 μm can be lowered more than twofold.

36 MATERIALS SCIENCE↗

An investigation of the electronic, structural and magnetic properties of the ruddlesden-popper phase Sr{sub 3}RuCoO{sub 7}

The structural, magnetic and electronic properties of the Ruddlesden-Popper material Sr{sub 3}CoRuO{sub 7} have been investigated. Examination of the dc and ac magnetic susceptibility demonstrates that Sr{sub 3}CoRuO{sub 7} exhibits a spin glass transition at 40 K and a magnetic transition at 140 K. Variable-temperature neutron powder diffraction experiments showed no evidence of magnetic diffraction peaks down to 5 K. This suggests the transition at 140 K is a result of short range magnetic order or magnetic clustering of the Co/Ru spins. Sr{sub 3}CoRuO{sub 7} is semiconducting and Mott variable range hopping behaviour is observed below 240 K. - Graphical abstract: Short range antiferromagnetic order is observed below ∼ 140 K in Sr{sub 3}CoRuO{sub 7} followed by spin glass behaviour at 40 K. Display Omitted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Gastrointestinal citrate absorption in nephrolithiasis

Gastrointestinal absorption of citrate was measured in stone patients with idiopathic hypocitraturia to determine if citrate malabsorption could account for low urinary citrate. Citrate absorption was measured directly from recovery of orally administered potassium citrate (40 mEq.) in the intestinal lavage fluid, using an intestinal washout technique. In 7 stone patients citrate absorption, serum citrate levels, peak citrate concentration in serum and area under the curve were not significantly different from those of 7 normal subjects. Citrate absorption was rapid and efficient in both groups, with 96 to 98% absorbed within 3 hours. The absorption of citrate was less efficient from a tablet preparation of potassium citrate than from a liquid preparation, probably due to a delayed release of citrate from wax matrix. However, citrate absorption from solid potassium citrate was still high at 91%, compared to 98% for a liquid preparation. Thus, hypocitraturia is unlikely to be due to an impaired gastrointestinal absorption of citrate in stone patients without overt bowel disease.

Non-NASA Center↗

Activation conductivity in HgTe/CdHgTe quantum wells at integer Landau level filling factors: Role of the random potential

Shubnikov-de Haas oscillations are studied in 8-nm-wide HgTe/CdHgTe quantum wells with an electron concentration of (1.7–13) × 10{sup 11} cm{sup –2} in the temperature range from 1.6 to 40 K. The gaps between Landau levels and the quantum relaxation time are determined from the temperature dependence of the oscillation amplitude at integer filling factors. The experimental gap values are found to be in good agreement with the results of the single-particle calculation of the level energies using the 8-band Kane model. The experimental widths of the density of states are indicative of profound screening of the exchange interaction in HgTe/CdHgTe quantum wells.

36 MATERIALS SCIENCE↗

Comprehensive Baseline Environmental Monitoring of an Interim Legacy Waste Store in Arid Zone Australia - 20062

Radionuclide containing soil and rubble from the clean-up of a former uranium, thorium and rare earth minerals processing research facility carried out in the early 50's and 60's is currently stored at the Woomera Test Range in South Australia awaiting final disposal. Prior to developing a final disposal pathway commensurate with waste acceptance criteria, a comprehensive baseline environmental monitoring has been carried out to establish the background radiation levels. The survey included in situ gamma scanning of the surface soil ({sup 238}U, {sup 232}Th, {sup 40}K), a laboratory analysis of 86 soil samples (from 0-20 cm depth), which involved XRF measurements (U, Th, and rare earth metals) and spectroscopic analysis ({sup 238}U, {sup 232}Th, {sup 226}Ra and daughter nuclides). A time series of radon concentration measurements in air was established, while soil radon ({sup 222}Rn) and thoron ({sup 220}Rn) flux measurements were undertaken at 18 different locations. The 2018 comprehensive baseline survey demonstrated radiation levels in the immediate vicinity of the Woomera interim waste store are typical background values of soil and rock. No contamination was detected. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Radiation-chemical processes leading to origination and accumulation of oxygen in the Earth’s atmosphere

The role of natural radioactivity in the formation of the oxygen atmosphere of the Earth is discussed. The origination of oxygen in the free state in the hydrosphere and atmosphere is associated with the radiolysis of the water of the World ocean under the irradiation of radio active isotopes {sup 40}K, {sup 235}U, {sup 238}U, and {sup 232}Th. The calculations showed that within the last 3.8 billion years the total weight of oxygen, which could be formed due to this process, is about 7.4•10{sup 17} kg, i.е., the value of the same order as the oxygen content in the modern atmosphere of the Earth. The Ocean was an intermediate collector and provided the nucleation of new forms of biological life with oxygen respiration. The consecutive transformation of the Earth’s atmosphere with a gradual increase in the oxygen content became the result of photosynthesis in algae and green plants and thus opened a way to the origination of complicated forms of the life.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Effect of the Composition of a Carrier Gas during the Growth of a Mn delta-Layer on the Electrical and Magnetic Properties of GaAs Structures

The effect of the arsine content (from 0 to 8 μmol), supplied to a reactor together with hydrogen, on the formation of delta-doped gallium-arsenide structures by the pulsed laser sputtering of a Mn target is investigated. It is found that an arsine molar fraction of ~2.5 μmol in the reactor atmosphere during the formation of a Mn delta-doped GaAs layer allows one to obtain single-crystal epitaxial structures with the lowest layer resistance and a ferromagnetic-paramagnetic phase transition temperature of about 40 K. Increasing the arsine content to 8 μmol or the absence of arsine in a hydrogen flow leads to a significant increase in the layer resistance in the temperature range below 150 K and a decrease in the Curie temperature. In the first case, this may be due to partial compensation of the hole conductivity by donor-type defects formed as a result of an excess of arsenic on the growing surface (arsenic atoms in Ga positions or in interstitial positions). In the second case, when no arsine is supplied to the reactor, the growth surface is likely to be enriched with gallium atoms, which makes the incorporation of Mn into the Ga sublattice difficult.

36 MATERIALS SCIENCE↗

Causes of the Metamagnetism in a Disordered EuMn{sub 0.5}Co{sub 0.5}O{sub 3} Perovskite

The magnetic properties of the EuMn{sub 0.5}Co{sub 0.5}O{sub 3} perovskite synthesized under various conditions are studied in fields up to 140 kOe. The sample synthesized at T = 1500°C is shown to exhibit a metamagnetic phase transition, which is irreversible below T = 40 K, and the sample synthesized at T = 1200°C demonstrates the field dependence of magnetization that is typical of a ferromagnet. Both samples have T{sub C} = 123 K and approximately the same magnetization in high magnetic fields. The metamagnetism is assumed to be related to a transition from a noncollinear ferromagnetic phase to a collinear phase, and the presence of clusters with ordered Co{sup 2+} and Mn{sup 4+} ions leads to ferromagnetism. The noncollinear phase is formed due to the competition between positive Co{sup 2+}–Mn{sup 4+} and negative Mn{sup 4+}–Mn{sup 4+} and Co{sup 2+}–Co{sup 2+} interactions, which make almost the same contributions, and to the existence of a high magnetic anisotropy.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Alternative Energy: Production of H{sub 2} by Radiolysis of Water in the Rocky Cores of Icy Bodies

We applied a model of radiolysis in earthly rock–water mixtures to several known or suspected ocean worlds: Enceladus, Ceres, Europa, Titania, Oberon, Pluto, and Charon. In this model, radiation emitted by the long-lived radionuclides ({sup 40}K, {sup 232}Th, {sup 235}U, and {sup 238}U) contained in the ordinary chondrite-like rocks is partly absorbed by the water permeating the material of each body’s core. The physical and chemical processes that follow release molecular hydrogen (H{sub 2}), which is a molecule of astrobiological interest. We compared the calculated production of H{sub 2} by radiolysis in each body’s core to published estimates of production by serpentinization. This study presents production calculations over 4.5 Gyr for several values of rock porosity. We found that radiolysis can produce H{sub 2} quantities equivalent to a few percent of what is estimated from serpentinization. Higher porosity, which is unlikely at the scale of a body’s entire core but possible just under the seafloor, can increase radiolytic production by almost an order of magnitude. The products of water radiolysis also include several oxidants, allowing for production of life-sustaining sulfates. Though previously unrecognized in this capacity, radiolysis in an ocean world’s outer core could be a fundamental agent in generating the chemical energy that could support life.

79 ASTRONOMY AND ASTROPHYSICS↗

Development of Processing Technology for Radioactively Contaminated Water at Chernobyl Nuclear Power Plant - 19656

During the operation of the Chernobyl Nuclear Power Plant, distillation by evaporation was the main method for processing radioactively contaminated water. When the plant was decommissioned, the evaporation facility was mothballed and floor drain treatment was suspended in 2016. At present, the existing tanks with the capacity of 26,000 m{sup 3} are more than 60% full with radioactively contaminated floor drains, which requires alternative processing methods. The current process flow for radioactive waste management at State Specialized Enterprise 'Chernobyl NPP' includes processing of accumulated liquid radioactive wastes at a liquid radioactive wastes processing plant. Under the processing technology, liquid radioactive waste is immobilized at the plant by cementation and the resulting solid radioactive waste is then buried in a near-surface storage. Key factors for the selection of alternative radioactively contaminated water processing methods are the possibility to clear the processed water (no control monitoring), which requires the same degree of processing as for drinking water, and minimization of radioactive waste generation due to the lack of free space for solid waste disposal in the near-surface storage. Floor drains that require processing contain radionuclides such as {sup 137}Cs, {sup 90}Sr, {sup 60}Co and {sup 40}K. The current level of the total beta and gamma activity is about 4*105 Bq/kg. The following criteria are set for the Chernobyl NPP site for water to be disposed to the sewerage system: - Max. 37 Bq/kg for the total beta and gamma containing radionuclide activity; - Max. 0.7 Bq/kg for the total alpha containing radionuclide activity. METOIL produces inorganic sorbents for removing radionuclides from liquids and develops sorbent-based technology for a variety of applications related to liquid radioactive waste processing. In 2017-2018, experts from the Chernobyl NPP and METOIL ran several joint laboratory tests to evaluate the efficiency of inorganic sorbents made by METOIL for processing floor drains at the Chernobyl NPP. The test procedure included treatment of radioactively contaminated water in a two-stage sorption process: static sorption (sorbents are mixed in a liquid) and dynamic sorption (the liquid is filtered through a sorbent column). NIKET and MODIKS sorbents were provided for the tests. The results of the test measurements showed that the total alpha containing radionuclide activity is less than 0.026 Bq/kg and the total beta and gamma containing radionuclide activity is 9.2 Bq/kg. The physical and chemical parameters after processing also met the water disposal criteria. High sorption capacity of the sorbents used for the tests allows processing hundreds of water volumes with just one sorbent volume. At present, preparations are underway for full-scale tests at a pilot plant with a capacity of minimum 10 m{sup 3}/day. At a later stage, spent sorbents may be immobilized by inclusion into the cement matrix, which will substantially reduce the amount of radioactive waste to be buried. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗