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At least 613 records · Page 34

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↗

Small Stirling dynamic isotope power system for robotic space missions

The design of a multihundred-watt Dynamic Isotope Power System (DIPS), based on the U.S. Department of Energy (DOE) General Purpose Heat Source (GPHS) and small (multihundred-watt) free-piston Stirling engine (FPSE), is being pursued as a potential lower cost alternative to radioisotope thermoelectric generators (RTG's). The design is targeted at the power needs of future unmanned deep space and planetary surface exploration missions ranging from scientific probes to Space Exploration Initiative precursor missions. Power level for these missions is less than a kilowatt. The incentive for any dynamic system is that it can save fuel and reduce costs and radiological hazard. Unlike DIPS based on turbomachinery conversion (e.g. Brayton), this small Stirling DIPS can be advantageously scaled to multihundred-watt unit size while preserving size and mass competitiveness with RTG's. Stirling conversion extends the competitive range for dynamic systems down to a few hundred watts--a power level not previously considered for dynamic systems. The challenge for Stirling conversion will be to demonstrate reliability and life similar to RTG experience. Since the competitive potential of FPSE as an isotope converter was first identified, work has focused on feasibility of directly integrating GPHS with the Stirling heater head. Thermal modeling of various radiatively coupled heat source/heater head geometries has been performed using data furnished by the developers of FPSE and GPHS. The analysis indicates that, for the 1050 K heater head configurations considered, GPHS fuel clad temperatures remain within acceptable operating limits. Based on these results, preliminary characterizations of multihundred-watt units have been established.

Bents, D. J.↗

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↗

Steady Nuclear Combustion in Rockets

The astrophysical theory of stationary nuclear reactions in stars is applied to the conditions that would be met in the practical engineering cases that would differ from the former, particularly with respect to the much lower combustion pressures, dimensions of the reacting volume, and burnup times. This application yields maximum rates of hear production per unit volume of reacting gas occurring at about 10(exp 8) K in the cases of reactions between the hydrogen isotopes, but yields higher rates for heavier atoms. For the former, with chamber pressures of the order of 100 atmospheres, the energy production for nuclear combustion reaches values of about 10(exp 4) kilocalories per cubic meter per second, which approaches the magnitude for the familiar chemical fuels. The values are substantially lower for heavier atoms, and increase with the square of the combustion pressure. The half-life of the burnup in the fastest reactions may drop to values as low as those for chemical fuels so that, despite the high temperature, the radiated energy can remain smaller than the energy produced, particularly if an inefficiently radiating (i.e., easily completely ionized reacting material like hydrogen), is used. On the other hand, the fraction of completely ionized particles in the gases undergoing nuclear combustion must not exceed a certain upper limit because the densities (approximately 10(exp -10) grams per cubic centimeter)) lie in the range of high vacua and only for the previously mentioned fraction of nonionized particles can mean free paths be retained small enough so that the chamber diameters of several dozen meters will suffice. Under these conditions it appears that continuously maintained stable nuclear reactions at practical pressures and dimensions are fundamentally possible and their application can be visualized as energy sources for power plants and propulsion units.

Saenger, E.↗

Envelope structure on 700 AU scales and the molecular outflows of low-mass young stellar objects

Aperture synthesis observations of HCO+ J = 1-0, 13CO 1-0, and C18O 1-0 obtained with the Owens Valley Millimeter Array are used to probe the small-scale (5" approximately 700 AU) structure of the molecular envelopes of a well-defined sample of nine embedded low-mass young stellar objects in Taurus. The interferometer results can be understood in terms of: (1) a core of radius approximately or less than 1000 AU surrounding the central star, possibly flattened and rotating; (2) condensations scattered throughout the envelope that may be left over from the inhomogeneous structure of the original cloud core or that may have grown during collapse; and (3) material within the outflow or along the walls of the outflow cavity. Masses of the central cores are 0.001-0.1 M (solar), and agree well with dust continuum measurements. Averaged over the central 20" (3000 AU) region, an HCO+ abundance of 4 x 10(-8) is inferred, with a spread of a factor of 3 between the different sources. Reanalysis of previously presented single-dish data yields an HCO+ abundance of (5.0 +/- 1.7) x 10(-9), which may indicate an average increase by a factor of a few on the smaller scales sampled by the interferometer. Part of this apparent abundance variation could be explained by contributions from extended cloud emission to the single-dish C18O lines, and uncertainties in the assumed excitation temperatures and opacities. The properties of the molecular envelopes and outflows are further investigated through single-dish observations of 12CO J = 6-5, 4-3, and 3-2, 13CO 6-5 and 3-2, and C18O 3-2 and 2-1, obtained with the James Clerk Maxwell and IRAM 30 m telescopes, along with the Caltech Submillimeter Observatory. Ratios of the mid-J CO lines are used to estimate the excitation temperature, with values of 25-80 K derived for the gas near line centre. The outflow wings show a similar range, although Tex is enhanced by a factor of 2-3 in at least two sources. In contrast to the well-studied L1551 IRS 5 outflow, which extends over 10' (0.4 pc), seven of the remaining eight sources are found to drive 12CO 3-2 outflows over < or = 1' (0.04 pc); only L1527 IRS has a well-developed outflow of some 3'(0.12 pc). Estimates are obtained for the outflow kinetic luminosity, Lkin, and the flow momentum rate, FCO, applying corrections for line opacity and source inclination. The flow force FCO correlates with the envelope mass and with the 2.7 mm flux of the circumstellar disk. Only a weak correlation is seen with Lbol, while none is found with the relative age of the object as measured by integral Tmb(HCO+ 3-2)dV/Lbol. These trends support the hypothesis that outflows are driven by accretion through a disk, with a global mass infall rate determined by the mass and density of the envelope. The association of compact HCO+ emission with the walls of the outflow cavities indicates that outflows in turn influence the appearance of the envelopes. It is not yet clear, however, whether they are actively involved in sweeping up envelope material, or merely provide a low-opacity pathway for heating radiation to reach into the envelope.

NASA Discipline Exobiology↗