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At least 541 records · Page 30

Active anaerobic methane oxidation and sulfur disproportionation in the deep terrestrial subsurface

Abstract Microbial life is widespread in the terrestrial subsurface and present down to several kilometers depth, but the energy sources that fuel metabolism in deep oligotrophic and anoxic environments remain unclear. In the deep crystalline bedrock of the Fennoscandian Shield at Olkiluoto, Finland, opposing gradients of abiotic methane and ancient seawater-derived sulfate create a terrestrial sulfate-methane transition zone (SMTZ). We used chemical and isotopic data coupled to genome-resolved metaproteogenomics to demonstrate active life and, for the first time, provide direct evidence of active anaerobic oxidation of methane (AOM) in a deep terrestrial bedrock. Proteins from Methanoperedens (formerly ANME-2d) are readily identifiable despite the low abundance (≤1%) of this genus and confirm the occurrence of AOM. This finding is supported by 13C-depleted dissolved inorganic carbon. Proteins from Desulfocapsaceae and Desulfurivibrionaceae, in addition to 34S-enriched sulfate, suggest that these organisms use inorganic sulfur compounds as both electron donor and acceptor. Zerovalent sulfur in the groundwater may derive from abiotic rock interactions, or from a non-obligate syntrophy with Methanoperedens, potentially linking methane and sulfur cycles in Olkiluoto groundwater. Finally, putative episymbionts from the candidate phyla radiation (CPR) and DPANN archaea represented a significant diversity in the groundwater (26/84 genomes) with roles in sulfur and carbon cycling. Our results highlight AOM and sulfur disproportionation as active metabolisms and show that methane and sulfur fuel microbial activity in the deep terrestrial subsurface.

59 BASIC BIOLOGICAL SCIENCES↗

Volume 4: Detection Systems and Ultra-Cold Neutrons

As part of the Sustaining and Enhancing Nuclear Science (SENSe) initiative at Oak Ridge National Laboratory (ORNL), the prospect of adding new detection systems to support High Flux Isotope Reactor (HFIR) operations and to advance scientific research has prompted many ideas and discussions regarding potential features, configurations, locations, and applications. A working group of ORNL staff members was organized to further develop the concepts and recommending one or more configurations to best support future HFIR operations and scientific capacities and to provide order-of-magnitude cost estimates and timing. The areas of investigation included fast access detection systems, non-scattering beamline instruments, shielded detection instruments, and an ultracold neutron source. In each case, the focus was to develop world leading capabilities that would be unmatched by any other facility.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Wavelength-Selective Reactivity of Iron(III) Halide Salts in Photocatalytic C–H Functionalization

The utility of halogen radicals in hydrocarbon functionalization extends from early examples of photochemical halogenation to recent reports using photoredox catalysis with iridium complexes and simple transition metal salts such as FeCl 3 . The majority of these methods (uncatalyzed and iron-catalyzed) require UV light (λ ≤ 390 nm), and systematic efforts to enable the use of visible light remain valuable. We report the use of a simple Fe(III) salt that enables a C–H to C–C and C–N functionalization under visible light. The reactivity and selectivity profile using different light sources demonstrates wavelength-selective behavior, which was further investigated with deuterium kinetic isotope effect experiments and DFT calculations. These results show that control over the reactive intermediates in this iron-catalyzed reaction can be achieved through proper choice of the wavelength of irradiation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-rate heavy-ion tracking using MWPCs and PPACs with an Anti-Discharge Unit

This work reports on the development of two robust, heavy-ion beam tracking concepts operating at low pressure (< 15 Torr) for high rate applications (> 200 kHz). The first concept consists of a Multi-Wire Proportional Counter (MWPC) with a central anode consisting of 12 μm Au-plated Tungsten wires spaced 1 mm from each other. The anode grid is sandwiched between two segmented cathodes aligned orthogonally in the two dimensions for (x,y) particle localization. The second detector is a Parallel-Plate Avalanche Counter (PPAC) that uses the same readout geometry as the MWPC, but replaces the wire anode with a 150 nm silver layer deposited on both sides of a thin (< 1 mg/cm 2 ) polypropylene foil. Additionally, the bias circuitry for the PPAC anode central foil is equipped with an Anti-Discharge Unit (ADU) to prevent transitions from proportional operation to streamer formation, thereby avoiding damaging discharges. The localization capability of both detectors was tested with a low-rate alpha-particle source (241-Am). A position resolution of < 1 mm (FWHM) was achieved under stable, high-gas-gain (> 1000) operating conditions. Their performance in terms of detection efficiency as a function of the isotope charge (Z) was determined by irradiating the detectors with a cocktail beam (Z ≤ 15) with energy of ∼ 100 MeV/u. Full detection efficiency is maintained for all available fragments under optimal operational conditions (i.e., voltage bias). Full detection efficiency was achieved at rates above 200 kHz by irradiating the detectors with a 1 cm diameter 238 U beam at an energy of 143 MeV/u.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Neutron Scattering in High Magnetic Fields: Community Recommendations to Seize the Moment for Scientific Breakthroughs

Oak Ridge National Laboratory (ORNL) operates the world’s two most powerful neutron sources: the High Flux Isotope Reactor (HFIR) and the Spallation Neutron Source (SNS). These form a national user facility that provides neutron scattering instruments to probe and image static and dynamic properties of materials down to the atomic scale. Because the neutron carries a magnetic moment and the energies and wavelengths of neutrons match energy and length scales associated with magnetic materials, these facilities provide unique sensitivity to magnetism.

36 MATERIALS SCIENCE↗

Determining the leading-order contact term in neutrinoless double β decay

We present a method to determine the leading-order (LO) contact term contributing to the nn → ppe - e - amplitude through the exchange of light Majorana neutrinos. Our approach is based on the representation of the amplitude as the momentum integral of a known kernel (proportional to the neutrino propagator) times the generalized forward Compton scattering amplitude n ( p 1 ) n ( p 2 ) W + ( k ) → \( p\left({p}_1^{\prime}\right)p\left({p}_2^{\prime}\right){W}^{-}(k) \) , in analogy to the Cottingham formula for the electromagnetic contribution to hadron masses. We construct model-independent representations of the integrand in the low- and high-momentum regions, through chiral EFT and the operator product expansion, respectively. We then construct a model for the full amplitude by interpolating between these two regions, using appropriate nucleon factors for the weak currents and information on nucleon-nucleon ( NN ) scattering in the 1 S 0 channel away from threshold. By matching the amplitude obtained in this way to the LO chiral EFT amplitude we obtain the relevant LO contact term and discuss various sources of uncertainty. We validate the approach by computing the analog I = 2 NN contact term and by reproducing, within uncertainties, the charge-independence-breaking contribution to the 1 S 0 NN scattering lengths. While our analysis is performed in the \( \overline{\mathrm{MS}} \) scheme, we express our final result in terms of the scheme-independent renormalized amplitude \( {\mathcal{A}}_{\nu}\left(\left|\mathbf{p}\right|,\left|\mathbf{p}^{\prime}\right|\right) \) at a set of kinematic points near threshold. We illustrate for two cutoff schemes how, using our synthetic data for \( {\mathcal{A}}_{\nu } \) , one can determine the contact-term contribution in any regularization scheme, in particular the ones employed in nuclear-structure calculations for isotopes of experimental interest.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Survey of Dynamic Mode Decomposition Methods

Dynamic mode decomposition (DMD) is a data-driven reduced order modeling (ROM) technique used for dynamic systems. The widely adopted algorithm was first introduced and demonstrated on fluid flow data by Schmid. In recent years, various other fields, such as nuclear engineering, have begun to adopt this method. For example, DMD has been used for estimating α-eigenvalues, as an ROM for pulsed neutron problems, for predicting isotopic composition in burnup calculations, as acceleration techniques for iterative methods, and in capturing dynamic behaviors in molten salt reactor transients. This report seeks to demonstrate the capabilities and limits of the standard DMD algorithm, and identify problem spaces where variants may be better suited. The primary variant this report considers is Multi-Resolution DMD (mrDMD). Because this serves as a survey, synthetically produced data is used in lieu of simulation results. The remainder of this report will go into detail on the DMD theory, outline the standard DMD and mrDMD algorithms, present test cases highlighting the applicability of each, and finally present a discussion on how to determine the best suited algorithm for a given problem. All calculations performed in this report are carried out using the open source DMD library, PyDMD.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Application of Gaussian Bayes classifier to differentiate chlorine-based chemical agents

The Portable Isotopic Neutron Spectroscopy (PINS) is a commercialized system developed by Idaho National Laboratory (INL) to examine chemical warfare agents (CWA) non-destructively, utilizing Prompt Gamma Neutron Activation Analysis (PGNAA) techniques. The PINS system takes advantage of a high-resolution gamma-ray spectrum from a mechanically-cooled high-purity germanium (HPGe) detector. One of the difficult technical challenges is to discriminate the chlorine-based chemical agents. Especially, CN, CNB, CNS and CG have similar chemical compositions to make it hard to discriminate them with a higher confidence. Current identification algorithms for PINS systems with 252-Cf sources have been improved and updated continuously as more field data became available, and new algorithms was studied to complement the current algorithms by adopting the Gaussian Bayes classifier. These new algorithms were intended to be applied to a subset of chlorine-based chemical agents, and their main goal is discriminate CN, CNB, CNS and CG with their ratios of the chlorine neutron inelastic 1763keV peak to the chlorine thermal neutron capture 1959keV peak, which is referred to as the “Cl i/c” or “clic” ratio in this study. The Cl i/c ratios were assumed to follow Gaussian distributions with the means and the standard deviations unique to their corresponding chemical agents. The prior probabilities of these four chemical agents were optimized with a collection of field data to achieve the best performance in terms of precision or positive predictive value (PPV). Finally, their posterior probabilities as functions of the Cl i/c ratio were implemented in the current version of PINS analysis software in order to be tested with more field data.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Purification of legacy Ra-226 from ingrown Pb-210 using cation exchange chromatography

With the growing interest in using radium-226 (Ra-226) as a source material to produce essential radionuclides for targeted alpha therapies, the global demand for Ra-226 has surged, rendering its acquisition difficult. The shortage necessitates the exploration of alternative pathways to obtain this isotope beyond traditional commercial vendors. Legacy radium sources remain widespread due to Ra-226’s historical use but require the removal of ingrown daughter products to obtain a pure Ra-226 product. In conclusion, a straightforward and effective purification method for legacy Ra-226 ampoules has been developed using cation exchange chromatography, enabling the reliable conversion of legacy materials into high-purity Ra-226 solutions.

and nuclear chemistry↗

Age determination of a 75 Se gamma radiography source for nuclear forensics

Here, two methods were used to evaluate the age of 75 Se sealed source material. Both methods utilized gamma spectroscopy to determine the quantity of parent 75 Se present, but they differed in the technique used to determine the quantity of daughter 75 As. In one method, 75 As was quantified using inductively coupled plasma-mass spectrometry (ICP-MS) after using chromatographic techniques to separate the parent and daughter isotopes. In the other method, total As was measured using optical emission spectroscopy (OES), which did not require separation prior to measurement. The OES method was faster and gave slightly lower uncertainties, but required more daughter material to be present because of higher concentration requirements, making it unsuitable for young material. Both methods are hampered by the monoisotopic nature of As, but still gave reasonable model ages that were in agreement with each other.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Preliminary investigation of an uncertainty budget for uranium isotope ratio analysis using a liquid sampling—atmospheric pressure glow discharge—orbitrap mass spectrometer system

The liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source has proven to be an effective analysis tool for making uranium isotope ratio measurements when coupled to high-resolution mass spectrometers, such as the Orbitrap. While previous studies have shown the capabilities of the LS-APGD for isotope ratio determination, a systematic evaluation of the measurement uncertainty of the technique has not been conducted. To this end, the International Standards Organizations (ISO) guidelines to the expression of uncertainty in measurement (GUM analysis) have been applied to generate an uncertainty budget. For this work, a preliminary assessment derived from the GUM analysis was performed. The uncertainty in the instrument blank determination has been identified as a primary factor contributing to measurement uncertainty for the LS-APGD-Orbitrap method. These findings for the specific test case of uranium isotopic analysis will be invaluable in applications across the breadth of isotope ratio mass spectrometry performed on this unique instrumental platform.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

First direct 7 Be electron-capture $\mathrm{Q}$-value measurement toward high-precision searches for neutrino physics beyond the Standard Model

Here, we report the first direct measurement of the nuclear electron-capture (EC) decay Q value of 7 Be → 7 Li via high-precision Penning trap mass spectrometry (PTMS). This was performed using the LEBIT Penning trap located at the National Superconducting Cyclotron Laboratory/Facility for Rare Isotope Beams (NSCL/FRIB) using the newly commissioned Batch-Mode Ion-Source (BMIS) to deliver the unstable 7 Be + samples. With a measured value of Q EC = 861.963(23) keV, this result is three times more precise than any previous determination of this quantity. This improved precision and accuracy of the 7 Be EC decay Q value is critical for ongoing experiments that measure the recoiling nucleus in this system as a signature to search for beyond the Standard Model (BSM) neutrino physics using 7 Be-doped superconducting sensors. This experiment has extended LEBIT capabilities, using the first low-energy beam delivered by BMIS at FRIB for PTMS, as well as measuring the lightest-mass isotopes so far with LEBIT.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Proven Technologies for the Solidification of Complex Liquid Radioactive Waste (LRW): Global Case Studies of Applications and Disposal Options - 20424

Legacy radioactive waste streams from the Cold War still exist and newly generated waste streams from nuclear power plants and research institutes go untreated and expose environmental hazards at many nuclear sites. The nature of the waste is diverse, depending upon the source or the process from which it originated. The most problematic waste streams include complex liquids such as organic (tri-butyl-phosphate TBP) solutions contaminated with Pu and U isotopes, mixed sludge types, high acid radioactive waste, H-3 contaminated organic and aqueous streams, etc. Technological, environmental and economic challenges exist for the treatment and disposal of such waste streams. A proven technology that has been applied to LRW on a global basis provides one option as a low-cost solution to legacy streams and small volume, highly complex LRW frequently found during decommissioning at nuclear power plants and weapons sites. The engineered polymer technology from Nochar, USA, is capable of solidifying standard and highly complex LLW and ILW waste streams for interim or final storage, or for incineration. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Alpha Decay Chains as Thermal Power Sources: Analysis and Applications for RTGs

Radioactive sources can provide power in remote and environmentally harsh locations such as the arctic or space. The generators powered by such sources are rugged and can withstand extreme temperatures, lack of sunlight, and require no human intervention for multiple years. Radioisotopes are used in thermoelectric generators to provide power at remote sites and deep in space. Isotopes like Pu-238, Cm-244, and Am-241 are used in these generators by NASA for power in space probes and spacecrafts. These power sources deliver a steady supply of energy over extended periods of time. Alpha particles created during decay do not travel far in a material. Their kinetic energy is transferred to heat that we can then convert into energy. Unlike beta and gamma decay, the slower-moving alpha particles stop in the material, making their energy available for use. Energy from these natural decay processes provides a reliable source of power. Spontaneous fission is rare and unreliable, and unlike induced fission processes, alpha decay occurs naturally and does not require external management or ignition. The ideal properties of an isotope for use as a power source depend upon the intended use. For use in an Arctic research base over a period of several years, but less than a decade, an isotope that provides high power output over a shorter lifespan may be the most suitable option. Whereas, for deep space missions where a consistent power source for decades or perhaps more than 100 years is needed that would require a very different isotope. One with a much longer half-life that would provide consistent power throughout that time and survive in that state in for these extended periods of time. These examples represent two extreme sides in terms of time frames. By analyzing the power produced by different radioactive decay processes over time, we can evaluate the suitability of various isotope decay chains for specific uses. Some unstable isotopes undergo a series of radioactive decays, transforming into different isotopes at each step and resulting in a stable isotope. The lists of isotopes in these decay processes are known as decay chains. Some of these chains, illustrated in the figures below, are currently being investigated for use in radioisotope thermoelectric generators (RTGs) designed for a range of operational durations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Improved high-precision mass measurements of mid-shell neon isotopes

New mass values measured with the TITAN MR-TOF-MS are reported for the short-lived isotopes 24-26 Ne, produced at TRIUMF's ISAC facility using a uranium carbide target and cold FEBIAD ion source. A least-squares adjustment within the framework of the Atomic Mass Evaluation was performed and the improved precision of the new mass values is highlighted. The improved mass accuracy in this N = 14mid-shell region can also point to the refinement in values of the charge radii. By reducing the mass uncertainty of isotopes, their contribution of the mass shift uncertainty in laser spectroscopy can be negated. The work is part of developments for reaching the N = 20 Island of Inversion, where high molecular contamination hinders mass measurements of the neon isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Summary of Forensic Examinations in Support of Breach Sealed Source Event at Harborview Medical Facility on 2 May 2019

On May 2, 2019, International Isotopes, Inc. (INIS), a subcontractor to Triad National Security, LLC (contractor for Los Alamos National Laboratory) breached a sealed radioactive source containing ~2800 Ci of the radioactive isotope cesium-137 ( 137 Cs) at the University of Washington Harborview Research and Training (HRT) Building in downtown Seattle while attempting to recover the source for the National Nuclear Security Administration’s (NNSA’s) Off-site Source Recovery Program (OSRP). The breach of the source resulted in the contamination of 13 personnel, all 7 floors of the building, and a release of material to the environment. A summary of root and contributing causes of the event was investigated and published by a joint investigation team (JIT) co-led by NNSA and Triad National Security, LLC. That investigation was supported by forensics examinations provided by Pacific Northwest National Laboratory. This report summarizes the results of those forensic examinations.

61 RADIATION PROTECTION AND DOSIMETRY↗

Progress Toward Fast Decay Energy Spectroscopy for Actinide Analysis

Decay energy spectroscopy (DES) is an increasingly popular technique for measuring isotopic composition of actinide samples for nuclear safeguards applications. Current approaches for actinide DES utilize milligram-scale external gold absorbers (> 0.1 nJ/K) that are integrated with actinide samples through mechanical kneading and are thermally connected to microcalorimeters using indium or gold wire bonds. This leads to relatively slow sensor rise time and, consequently, limits counting speed to a few counts per second. We are developing faster metallic magnetic calorimeter-based DES by integrating actinide samples with magnetic sensor materials. This reduces signal rise time and enables high counting speed while maintaining the ability to knead the radioactive source with the absorber. We have measured signal rise time of 0.7 μs with a 1.5 mg external gold absorber using this approach. Here, we also demonstrated online DES operation using an Ortec DSPEC 50, a commercially available data acquisition system developed for semiconductor detectors.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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↗