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At least 883 records · Page 49

Reduced photothermal heating in diamonds enriched with H3 point defects

Solid-state laser refrigeration of semiconductors remains an outstanding experimental challenge. In this work, we show that, following excitation with a laser wavelength of 532 nm, bulk diamond crystals doped with H3 centers both emit efficient up-conversion (anti-Stokes) photoluminescence and also show significantly reduced photothermal heating relative to crystals doped with nitrogen–vacancy (NV) centers. The H3 center in diamond is a highly photostable defect that avoids bleaching at high laser irradiances of 10–70 MW/cm 2 and has been shown to exhibit laser action, tunable over the visible band of 500–600 nm. Here, the observed reduction of photothermal heating arises due to a decrease in the concentration of absorbing point defects, including NV-centers. These results encourage future exploration of techniques for H3 enrichment in diamonds under high-pressure, high-temperature conditions for the simultaneous anti-Stokes fluorescence cooling and radiation balanced lasing in semiconductor materials. Reducing photothermal heating in diamond through the formation of H3 centers also opens up new possibilities in quantum sensing via optically detected magnetic resonance spectroscopy at ambient conditions.

42 ENGINEERING↗

Development of Chemical Procedures for Isotope Harvesting: Separation of Trace Hafnium from Tungsten

The separation of trace hafnium from bulk tungsten alloys is of interest for isotope harvesting at the National Superconducting Cyclotron Laboratory and the Facility for Rare Ion Beams because 172 Hf, the parent of 172 Lu, accumulates in tungsten alloy beam blockers at these facilities. In this work, a procedure for the separation of trace hafnium from a bulk tungsten alloy (454 g) was established using tracer isotopes ( 175 Hf, 88 Zr, 173 Lu, and 88 Y). Here, the procedure employed dissolution in an HF–HNO 3 solution followed by a calcium fluoride precipitation, and then extraction chromatography was used for more selective separation steps. Two stages of column separations using LN resin (HDEHP based) and TRU resin (CMPO based) were performed. Gamma-ray spectroscopy and mass spectrometry were used to analyze the final hafnium sample and follow the steps in the chemical processing. Furthermore, the final recovery of hafnium was high (90 ± 8)%, and the mass of tungsten and other transition metals was reduced to near background levels (as determined by ICP-MS of the blank acid solutions). Zirconium follows hafnium quantitatively in this procedure; there was no detectable 173 Lu in the final hafnium sample.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Emission Spectra of Uranium Particulates at High Temperature

The emission spectrum of micron-scale uranium particulates at high temperatures in the ultraviolet, visible, and near-infrared spectral regions is investigated using a heterogeneous shock tube. Temperatures from 3000 to 9000 K are characterized in an inert argon environment and with incremental amounts of added oxygen. Atomic line spectra do not emerge above the continuum emission spectrum until between 4500 and 5000 K in pure argon, and 6100 and 6600 K in 1% oxygen. For 5% oxygen, however, the threshold for atomic emission drops below 3800 K. Uranium monoxide molecular emission in the strongest visible band at 595.4 nm is not observed at any condition. Uncertainties in particle temperature determination in high-temperature shock tube environments are discussed, and limitations to such measurements are presented, such as those from experimental factors such as the powder loading method and expected detection limits of uranium species in relevant conditions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

MARSAME Radiological Release Report for Metal Items from Technical Area 53, Set 28

Environmental Protection and Compliance, Environmental Stewardship Group (EPC-ES) has evaluated the survey results for metal items from the Los Alamos Neutron Science Center (LANSCE) at Technical Area 53 (TA-53) and found that the metal items described in Table 1 of this report (identified by Radiation Protection [RP] Tracking Numbers) meet the criteria for unrestricted release under Department of Energy (DOE) Order 458.1 Chg 4, Radiation Protection of the Public and the Environment (DOE 2020) and can be recycled. This conclusion is based on the known history of the metal items and radiation survey data (see the completed RP-Form-031 LANSCE Metals Clearance Log [LANL 2021a] for each item in Attachment 1). Process knowledge indicates that items were released from radiological areas, including radiation areas, prior to the implementation of the 2000 metals moratorium. Therefore, the items are considered unencumbered and are not subject to the moratorium suspension on metal recycling from DOE facilities. Additionally, Los Alamos National Laboratory (LANL) has determined that there is no practical opportunity for internal DOE reuse of this metal. Process knowledge indicates that these metal items were unlikely to ever be in direct contact with the beam and thus are unlikely to have become activated. Surface contamination measurements (both total and removable) showed either no detectable radioactivity or activity levels within the range of background. All measurements for volumetric contamination were indistinguishable from background based on calculated decision limits. Additionally, all gamma isotopic surveys conducted for defense-in depth showed no identifiable gamma radiation from beam activation.

61 RADIATION PROTECTION AND DOSIMETRY↗

Matrix-Assisted Ionization of Molecular Uranium Species

Matrix-assisted ionization (MAI) demonstrates high sensitivity for a variety of organic compounds; however, few studies have reported the application of MAI for the detection and characterization of inorganic analytes. Trace-level uranium analysis is important in the realms of nuclear forensics, nuclear safeguards, and environmental monitoring. Traditional mass spectrometry methods employed in these fields require combinations of extensive laboratory chemistry sample preparation and destructive ionization methods. There has been recent interest in exploring ambient mass spectrometry methods that enable timely sample analysis and higher sensitivity than what is attainable by field-portable radiation detectors. Rapid characterization of uranium at nanogram levels is demonstrated in this study using MAI techniques. Mass spectra were collected on an atmospheric pressure mass spectrometer for solutions of uranyl nitrate, uranyl chloride, uranyl acetate, and uranyl oxalate utilizing 3-nibrobenzonitrile as the ionization matrix. The uranyl complexes investigated were detectable, and the chemical speciation was preserved. Sample analysis was accomplished in a matter of seconds, and limits of detection of 5 ng of uranyl nitrate, 10 ng of uranyl oxalate, 100 ng of uranyl chloride, and 200 ng of uranyl acetate were achieved. The observed gas-phase speciation was similar to negative-ion electrospray ionization of uranyl compounds with notable differences. Six matrix-derived ions were detected in all negative-ion mass spectra, and some of these ions formed adducts with the uranyl analyte. Subsequent analysis of the matrix suggests that these molecules are not matrix contaminants and are instead created during the ionization process.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Assessment of Modeling and Nuclear Data Needs for Active Neutron Interrogation

This document is the primary deliverable for a scoping study proposed to DOE National Laboratory Announcement Number LAB 19-2114 in the NNSA research area. The study supports user applications employing active neutron interrogation by providing a science plan to improve the modeling capability and the nuclear data that radiation transport codes use. Users rely on the accuracy of the elastic scattering and non-elastic cross-sections spanning thermal energies to 14 MeV (and higher in some cases) for modeling the neutron transport through complex geometries of materials potentially composed of many elements. While the elastic scattering cross-section data are accepted for all commonly occurring elements, the non-elastic cross-section data and the associated emission data include reaction channels that require attention. The study focused on the non-elastic reactions that emit secondary, also known as prompt, gammas with the premise that many users would benefit from improved modeling of these reactions. Many users develop material assay technologies based upon gamma signatures from radiative capture, inelastic scattering, and reactions on low-Z isotopes emitting multiple particles, so the nuclear data gaps, modeling deficiencies, and recommendations for addressing the shortfalls were assessed for these reactions. Fission gammas were excluded from this study because there are other efforts underway to address known shortfalls. Follow-on efforts that successfully execute the recommendations will tangibly improve to the ability to model gamma signatures and backgrounds for user applications, such as controlled substance detection, oil-well logging, and space exploration.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

MARSAME Radiological Release Report for Metal Items from Technical Area 53, Set 26

Environmental Protection and Compliance, Environmental Stewardship Group (EPC-ES) has evaluated the survey results for metal items from the Los Alamos Neutron Science Center (LANSCE) at Technical Area 53 (TA-53) and found that the metal items described in Table 1 of this report (identified by Radiation Protection [RP] Tracking Numbers) meet the criteria for unrestricted release under Department of Energy (DOE) Order 458.1 Chg 4, Radiation Protection of the Public and the Environment (DOE 2020) and can be recycled. This conclusion is based on the known history of the metal items and radiation survey data. None of the items in this report are located within radiological areas. Therefore, the items are considered unencumbered and are not subject to the moratorium suspension on metal recycling from DOE facilities. Additionally, Los Alamos National Laboratory (LANL) has determined that there is no practical opportunity for internal DOE reuse of this metal. Process knowledge indicates that these metal items were unlikely to ever be in direct contact with the beam and thus are unlikely to have become activated. Surface contamination measurements (both total and removable) showed either no detectable radioactivity or activity levels within the range of background. All measurements for volumetric contamination were indistinguishable from background based on calculated decision limits. Additionally, all gamma isotopic surveys conducted for defense-in depth showed no identifiable gamma radiation from beam activation.

54 ENVIRONMENTAL SCIENCES↗

Enhanced backscatter and unsaturated blue wavelength shifts in F-doped fused silica optical fibers exposed to extreme neutron radiation damage

Amorphous fused silica (a-SiO 2 ) optical fibers, with and without inscribed Bragg gratings, were interrogated using infrared (~1550 nm) optical backscatter reflectometry during ~25 days of intense neutron irradiation to a fast (energy > 0.1 MeV) neutron fluence of ~10 21 n/cm 2 , or ~1.5 atomic displacements per atom. The reflected light amplitudes in Ge-doped core telecommunications fiber dropped below detection limits (>15 dB attenuation) within 3 days of irradiation (~10 20 fast n/cm 2 ). Here, amplitudes from a pure silica core, F-doped silica cladding fiber reached equilibrium levels ~1.5–2 dB higher than pre-irradiation values, whereas Bragg gratings inscribed in the same fiber using a femtosecond laser (point-by-point method) suffered > 45 dB attenuation. Blue wavelength shifts were initially consistent with previous radiation-induced compaction models but increased linearly with increasing neutron fluence (no evidence of saturation) beyond 10 20 n/cm 2 and exceeded 0.6%, which corresponds to >1,000 °C drift if used to measure temperature changes.

36 MATERIALS SCIENCE↗

Interaction of Polymethyl Methacrylate with Boehmite-Filmed Aluminum Cladding Under Gamma Irradiation

This paper presents an overview of ongoing work to qualify the Advanced Test Reactor (ATR) driver fuel elements that have been affected by irradiation-degraded polymethyl methacrylate (PMMA) flux wands. Irradiation testing was performed on PMMA material in contact with aluminum clad material. The cladding was prefilmed with a boehmite oxide layer, an important feature of the ATR driver fuel. The effects on the boehmite layer due to gamma irradiation of the PMMA-aluminum clad system were investigated. PMMA embrittlement, followed by softening and degradation, occurred at high radiation levels. Adhesion between the cladding and irradiated PMMA was observed. Flow testing at prototypic ATR flow rates demonstrated the effective removal of the adhered material. Measurements of the boehmite layer thickness were performed, and Raman spectroscopy was utilized to detect the presence of boehmite in the irradiated PMMA material.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Primary radiation damage in bone evolves via collagen destruction by photoelectrons and secondary emission self-absorption

X-rays are invaluable for imaging and sterilization of bones, yet the resulting ionization and primary radiation damage mechanisms are poorly understood. Here we monitor in-situ collagen backbone degradation in dry bones using second-harmonic-generation and X-ray diffraction. Collagen breaks down by cascades of photon-electron excitations, enhanced by the presence of mineral nanoparticles. We observe protein disintegration with increasing exposure, detected as residual strain relaxation in pre-stressed apatite nanocrystals. Damage rapidly grows from the onset of irradiation, suggesting that there is no minimal ‘safe’ dose that bone collagen can sustain. Ionization of calcium and phosphorous in the nanocrystals yields fluorescence and high energy electrons giving rise to structural damage that spreads beyond regions directly illuminated by the incident radiation. Our findings highlight photoelectrons as major agents of damage to bone collagen with implications to all situations where bones are irradiated by hard X-rays and in particular for small-beam mineralized collagen fiber investigations.

36 MATERIALS SCIENCE↗

Reduced volume of diabetic pancreatic islets in rodents detected by synchrotron X-ray phase-contrast microtomography and deep learning network

The pancreatic islet is a highly structured micro-organ that produces insulin in response to rising blood glucose. Here we develop a label-free and automatic imaging approach to visualize the islets in situ in diabetic rodents by the synchrotron radiation X-ray phase-contrast microtomography (SRμCT) at the ID17 station of the European Synchrotron Radiation Facility. The large-size images (3.2 mm × 15.97 mm) were acquired in the pancreas in STZ-treated mice and diabetic GK rats. Each pancreas was dissected by 3000 reconstructed images. The image datasets were further analysed by a self-developed deep learning method, AA-Net. All islets in the pancreas were segmented and visualized by the three-dimension (3D) reconstruction. After quantifying the volumes of the islets, we found that the number of larger islets (=>1500 μm 3 ) was reduced by 2-fold (wt 1004 ± 94 vs GK 419 ± 122, P < 0.001) in chronically developed diabetic GK rat, while in STZ-treated diabetic mouse the large islets were decreased by half (189 ± 33 vs 90 ± 29, P < 0.001) compared to the untreated mice. Our study provides a label-free tool for detecting and quantifying pancreatic islets in situ. It implies the possibility of monitoring the state of pancreatic islets in vivo diabetes without labelling.

59 BASIC BIOLOGICAL SCIENCES↗

Millicharged relics reveal massless dark photons

The detection of massless kinetically-mixed dark photons is notoriously difficult, as the effect of this mixing can be removed by a field redefinition in vacuum. In this work, we study the prospect of detecting massless dark photons in the presence of a cosmic relic directly charged under this dark electromagnetism. Such millicharged particles, in the form of dark matter or dark radiation, generate an effective dark photon mass that drives photon-to-dark photon oscillations in the early universe. We also study the prospect for such models to alleviate existing cosmological constraints on massive dark photons, enlarging the motivation for direct tests of this parameter space using precision terrestrial probes.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Discovery of a bright extended X-ray jet in RGB J1512+020A

ABSTRACT We report the discovery of a bright, extended X-ray jet in the quasar RGB J1512+020A (z = 0.22). Chandra observations show the X-ray core and 13 arcsec (∼45 kpc projected) extended emission coincident with the radio jet. The jet stands out as one of brightest X-ray jets (LX ∼ 7 × 1043 erg s−1) at low redshift (z < 0.5) discovered so far, with remarkably large X-ray to radio luminosity ratios (LX/Lr up to ∼50). We identified four main components, two unresolved knots and two extended structures, one being the jet brightest feature (JBF). All jet features are also detected in ALMA archival observations. The radio, sub-mm to X-ray spectra of the two knots can be modelled with a single synchrotron component. For the two resolved structures, the ALMA data unveil a turnover of the low-energy continuum at ∼460 GHz. External Comptonization of cosmic microwave background photons can account for the observed X-ray emission if the jet speed remains highly relativistic, with bulk motion Γbulk > 15, up to tens of kiloparsec from the core. However, the comparison with the spectral energy distribution of similar X-ray detected jets shows that the alternative hypothesis of synchrotron emission from an additional population of ultra-high-energy electrons is also possible. We report a tentative (≳2σ) optical detection of the JBF in images of the Dark Energy Camera Legacy Survey. If confirmed, the optical emission should be either the low-energy tail of the radiative component responsible for the X-ray emission or a third, separate component.

79 ASTRONOMY AND ASTROPHYSICS↗

Rapid Sample Insertion/Extraction Systems for Gamma Irradiation

The Rapid Sample Insertion/Extraction System for Gamma Irradiation, otherwise known as the "rabbit" system, was a four-week long project which included many different aspects; from coding an Arduino to building PVC piping to 3-D printing the "rabbit" capsules. The "rabbit" system is a system of PVC piping that allows a quick and efficient transfer of materials into/out of one of the irradiation chambers in the Gamma Irradiation Facility (GIF) with the use of a 3-D printed "rabbit." This "rabbit" encapsulates material to be irradiated and carries it from a position outside of the irradiation chamber to the basket inside of the chamber. The main purpose of this system is to save time and provide more exact data without any delays that normally occur when a person has to enter the chamber, retrieve data, and then analyze the data. This system should take measurements and retrieve the data instantaneously. The way in which the "rabbit" is sent through the PVC piping is with an advanced bi-directional, high-throughput pneumatic system, or a shop vacuum cleaner. When the vacuum is set to blow or suck then the "rabbit" will be pulled through the PVC piping to its intended destination and will hit sensors along the sides of the tubing when it reaches the end of the piping. These sensors tell the Arduino that the "rabbit" is finished moving throughout the tubing and stops a timer. Another timer is used to see how long the "rabbit" is being irradiated so when the "rabbit" reaches the sensors in the basket in the irradiation chamber another timer is started and it ends when the sensors no longer detect the "rabbit," which means that it has begun its journey back to the starting point.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

MARSAME Radiological Release Report for Metal Items from TA 53, Set 20

EPC-ES has evaluated the survey results for metal items from the Los Alamos Neutron Science Center (LANSCE) and found that the metal items described in Table 1 of this report (identified by RP Tracking Numbers) meet the criteria for unrestricted release under DOE Order 458.1 Radiation Protection of the Public and the Environment (DOE 2020) and can be recycled. This conclusion is based on the known history of the metal items and on radiation survey data (see the completed RP-Form-031 LANSCE Metals Clearance Log for each item). None of the items in this report are located within radiological areas. Therefore, the items are considered unencumbered and are not subject to the moratorium suspension on metal recycling from Department of Energy facilities. Additionally, LANL has determined that there is no practical opportunity for internal DOE reuse or recycling of this metal. Process knowledge indicates that these metal items were unlikely to ever be in direct contact with the beam and thus are unlikely to have become activated. Surface contamination measurements (both total and removable) showed either no detectable radioactivity or activity levels within the range of background. All measurements for volumetric contamination were indistinguishable from background based on calculated decision limits. Additionally, all gamma isotopic surveys conducted for defense-in-depth showed no identifiable gamma radiation from beam activation.

54 ENVIRONMENTAL SCIENCES↗

MARSAME Radiological Release Report for Metal Items from TA 53, Set 22

EPC-ES has evaluated the survey results for metal items from the Los Alamos Neutron Science Center (LANSCE) and found that the metal items described in Table 1 of this report (identified by RP Tracking Numbers) meet the criteria for unrestricted release under DOE Order458.1 Radiation Protection of the Public and the Environment (DOE 2020) and can be recycled. This conclusion is based on the known history of the metal items and on radiation survey data (see the completed RP-Form-031 LANSCE Metals Clearance Log [LANL 2021a] for each item). None of the items in this report are located within radiological areas. Therefore, the items are considered unencumbered and are not subject to the moratorium suspension on metal recycling from Department of Energy facilities. Additionally, LANL has determined that there is no practical opportunity for internal DOE reuse or recycling of this metal. Process knowledge indicates that these metal items were unlikely to ever bein direct contact with the beam and thus are unlikely to have become activated. Surface contamination measurements (both total and removable) showed either no detectable radioactivity or activity levels within the range of background. All measurements for volumetric contamination were indistinguishable from background based on calculated decision limits. Additionally, all gamma isotopic surveys conducted for defense-in-depth showed no identifiable gamma radiation from beam activation.

36 MATERIALS SCIENCE↗