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At least 109 records · Page 6

Lithium indium diselenide — An advanced material for neutron detection

Here, this paper describes the synthesis, crystal growth, detector fabrication, radiation hardening studies, MCNP modeling, and characterization of lithium indium diselenide or LiInSe 2 . This newly-developed room temperature thermal neutron detector has semiconducting and scintillating properties and it is suitable for neutron detection application. LiInSe 2 was synthesized starting from elemental Li, In, Se in two steps due to high reactivity of Li. A single crystal of LiInSe 2 was grown using the Vertical Bridgman method. The room temperature band gap was found to be 2.8 eV using optical absorption measurements. Bulk resistivity was measured at ∼5 × 10 11 Ωcm. Photoconductivity measurements of LiInSe 2 wafers identified a peak in the photocurrent around 445 nm. Nuclear radiation detectors were fabricated from single crystal wafer and the responses to alpha particles at various biases were measured. The mobility-lifetime product was estimated. Gamma irradiation studies were performed with calculated absorbed doses ranging from 0.2126 to 21,262 Gy. The characterization of the two wafers for their scintillator performance was conducted after each irradiation. The gamma irradiation produced a reduction of the light yield that translated to a lower channel number for the centroid of alpha detection spectra. It also showed a considerable reduction of the decay time after the first irradiation. These are the first studies on gamma radiation hardening with this material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Effect of gamma-ray irradiation on the surface states of MOS tunnel junctions

Gamma-ray irradiation with doses up to 8 megarad produces no significant change on either the C(V) or the G(V) characteristics of MOS tunnel junctions with intermediate oxide thicknesses (40-60 A), whereas the expected flat-band shift toward negative electrode voltages occurs in control thick oxide capacitors. A simple tunneling model would explain the results if the radiation-generated hole traps are assumed to lie below the valence band of the silicon. The experiments also suggest that the observed radiation-generated interface states in conventional MOS devices are not due to the radiation damage of the silicon surface.

Ma, T. P.↗

Influence of metal ion complexation on the radiolytic longevity of butyramide extractants under direct dissolution conditions

The direct dissolution of volox-treated used nuclear fuel (UNF) into an organic solution—comprised of diluent and specialized extractants—poses a promising alternative to the traditional liquid-liquid solvent extraction approach to reprocessing UNF. However, moving to direct dissolution removes the presence of a concentrated nitric acid aqueous phase, which has been shown to significantly influence the radiolytic longevity of extractants in liquid-liquid solvent extraction flowsheets. With this in mind, and given the limited knowledge of radiation effects under direct dissolution conditions, we present a time-resolved and dose accumulation study on the impact of direct dissolution conditions on the radiolytic longevity of two candidate butyramide extractants—N,N-di-(2-ethylhexyl) butyramide (DEHBA) and N,N-di-(2-ethylhexyl)isobutyramide (DEHiBA)—in pre-equilibrated n-dodecane solvent in the presence and absence of process relevant metal ions, uranium and rhenium. Rhenium, and by extension technetium, extraction had little impact (=10%) on the overall radiolytic stability of these ligands, despite observed increases in chemical kinetic reactivity (>2×) of the corresponding complexes with the n-dodecane radical cation. Uranium-loading on the other hand, significantly improved the lifetime of both ligands (>30%) under gamma irradiation, with a greater stabilization observed for DEHBA over DEHiBA. This draft manuscript has been prepared in fulfillment of NTRD-MRWFD-2024 M3FT-24IN030101115.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Irradiation of dihydropyrimidines.

Gamma irradiation effect on dihydropyrimidines in aqueous solution and solid state, stressing conversion to unsaturated forms and ESR spectroscopy of free radicals

Bernhard, W.↗

Sterilization of N95 Respirators via Gamma Radiation: Comparison of Post-sterilization Efficacy

This study evaluated gamma irradiation for sterilization and reuse of two models of N95 respirators after gamma radiation sterilization as a method to increase availability of N95 respirators during a shortage. The Sandia National Laboratories Gamma Irradiation Facility was used to irradiate two different models of N95 filtering facepiece respirators at doses ranging from 0 kGy(tissue) to 50 kGy(tissue). The following tests were used to determine the efficacy of the respirator after irradiation sterilization: Ambient Aerosol Condensation Nuclei Counter Quantitative Fit Test, tensile test, strain cycling, oscillatory dynamic mechanical analysis, microscopic image analysis of fiber layers, and electrostatic field measurements. Both of the respirator models exhibited statistically significant changes after gamma irradiation as shown by the Quantitative Fit Test, electrostatic testing and the aerosol testing. The change in electrostatic capability of the filter reduced the efficiency of challenging particles near the 200 nm size by approximately 40-50%. Both tested respirators showed statistically significant changes associated with gamma sterilization. However, our results indicate that choices in materials and manufacturing methods to achieve N95 filtration lead to different magnitudes of damage when exposed to gamma radiation at sterilization relevant doses. This damage results in lower filtration performance. While our sample size (2 different types of respirators) was small, we did observe a change in electrostatic properties on a filter layer that coincided with the failure on the Quantitative Fit Test.

61 RADIATION PROTECTION AND DOSIMETRY↗

Sterilization of N95 Respirators via Gamma Radiation: Comparison of Post-sterilization Efficacy

This study evaluated gamma irradiation for sterilization and reuse of two models of N95 respirators after gamma radiation sterilization as a method to increase availability of N95 respirators during a shortage. The Sandia National Laboratories Gamma Irradiation Facility was used to irradiate two different models of N95 filtering facepiece respirators at doses ranging from 0 kGy(tissue) to 50 kGy(tissue). The following tests were used to determine the efficacy of the respirator after irradiation sterilization: Ambient Aerosol Condensation Nuclei Counter Quantitative Fit Test, tensile test, strain cycling, oscillatory dynamic mechanical analysis, microscopic image analysis of fiber layers, and electrostatic field measurements. Both of the respirator models exhibited statistically significant changes after gamma irradiation as shown by the Quantitative Fit Test, electrostatic testing and the aerosol testing. The change in electrostatic charge of the filter was correlated with a reduction in capturing particles near the 200 nm size by approximately 40-50%. Both tested respirators showed statistically significant changes associated with gamma sterilization. However, our results indicate that choices in materials and manufacturing methods to achieve N95 filtration lead to different magnitudes of damage when exposed to gamma radiation at sterilization relevant doses. This damage results in lower filtration performance. While our sample size (2 different types of respirators) was small, we did observe a change in electrostatic properties on a filter layer that coincided with the failure on the Quantitative Fit Test and reduction in aerosol filtering efficiency. Key Words: N95 respirators, respirators, airborne transmission, pandemic prevention, COVID-19, gamma sterilization

COVID-19↗

Radiolytic evaluation of a new technetium redox control reagent for advanced used nuclear fuel separations

Technetium is a problematic radioisotope for used nuclear fuel (UNF) and subsequent waste management owing to its high environmental mobility and coextraction in reprocessing technologies as the pertechnetate anion (TcO 4 - ). Consequently, several strategies are under development to control the transport of this radioisotope. A proposed approach is to use diaminoguanidine (DAG) for TcO 4 - and transuranic ion redox control. Although the initial DAG molecule is ultimately consumed in the redox process, its susceptibility to radiolysis is currently unknown under envisioned UNF reprocessing conditions, which is a critical knowledge gap for evaluating its overall suitability for this role. To this end, we report the impacts of steady-state gamma irradiation on the rate of DAG radiolysis in water, aqueous 2.0 M nitric acid (HNO 3 ), and in a biphasic solvent system composed of aqueous 2.0 M HNO 3 in contact with 1.5 M N,N-di-(2-ethylhexyl)isobutyramide (DEHiBA) dissolved in n-dodecane. In addition, we report chemical kinetics for the reaction of DAG with key transients arising from electron pulse radiolysis, specifically the hydrated electron (e aq - ), hydrogen atom (H ˙ ), and hydroxyl ( ˙ OH) and nitrate (NO 3 ˙ ) radicals. The DAG molecule exhibited significant reactivity with the ˙ OH and NO 3 ˙ radicals, indicating that oxidation would be the predominant degradation pathway in radiation environments. This is consistent with its role as a reducing agent. Steady-state gamma irradiations demonstrated that DAG is readily degraded within a few hundred kilogray, the rate of which was found to increase upon going from water to HNO 3 containing solutions and solvents systems. This was attributed to a thermal reaction between DAG and the predominant HNO 3 radiolysis product, nitrous acid (HNO 2 ), k(DAG + HNO 2 ) = 5480 ± 85 M -1 s -1 . Although no evidence was found for the radiolysis of DAG altering the radiation chemistry of the contacted DEHiBA/n-dodecane phase in the investigated biphasic system, the utility of DAG as a redox control reagent will likely be limited by significant competition with its degradation by HNO 2 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Hydrothermal corrosion of laser printed SiC fibers under extreme environment

We report SiC/SiC fiber composites are proposed cladding materials to improve the accident tolerance of commercial light water nuclear reactor fuel. To evaluate their viability, understanding the kinetics of corrosion under irradiation and high-temperature, high-pressure aqueous environment is critical. In the present work, the microstructure and mechanical properties of novel SiC fibers manufactured by Laser Chemical Vapor Deposition (LCVD) are introduced. The LCVD technology has control over microstructure and stoichiometry while allowing for high purity manufacturing, all key qualities needed in search of an optimum SiC fiber for nuclear energy applications. The isolated hydrothermal corrosion of commercially available carbon-rich Hi-Nicalon Type-S fibers is compared to the LCVD stoichiometric and LCVD silicon-rich fibers. Autoclave testing was carried out at 310°C and 14 MPa in the absence of irradiation. In a separate study, the effect of gamma irradiation on the fibers in the room-temperature environment was analyzed. It was observed from the experiments that the dissolution of the fibers was highly dependent on the stoichiometric ratio, fiber surface morphology and thermal pre-treatment of fibers. Contrary to previous findings, fiber dissolution was also visible under low-temperature gamma irradiation in aqueous environment with LCVD fibers showing lower dissolution.

36 MATERIALS SCIENCE↗

Impact of high-dose gamma-ray irradiation on electrical characteristics of N-polar and Ga-polar GaN p–n diodes

We investigate the impact of high-dose gamma-ray irradiation on the electrical performance of Ga-polar and N-polar GaN-based p-n diodes grown by metalorganic chemical vapor deposition. We compare the current density-voltage (J-V), capacitance-voltage (C-V), and circular transfer length method (CTLM) characteristics of the p-n diodes fabricated on Ga-polar and N-polar orientations before and after irradiation. The relative turn-on voltage increases for the Ga-polar diodes with increasing irradiation dose, while it increases initially and then starts to decrease for the N-polar diodes. The p-contact total resistance increases for Ga-polar and decreases for N-polar samples, which we attribute to the formation of point defects and additional Mg activation after irradiation. The J-V characteristics of most of the tested diodes recovered over time, suggesting the changes in the J-V characteristics are temporary and potentially due to metastable occupancy of traps after irradiation. X-ray photoelectron spectroscopy (XPS) and photoluminescence (PL) measurements reveal the existence of different types of initial defects and surface electronic states on Ga-polar and N-polar samples. Gallium vacancies (V Ga ) are dominant defects in Ga-polar samples, while nitrogen vacancies (V N ) are dominant in N-polar samples. The presence of a higher concentration of surface states on Ga-polar surfaces compared to N-polar was confirmed by calculating the band bending and the corresponding screening effect due to opposite polarization bound charge and ionized acceptors at the surface. The difference in surface stoichiometry in these two orientations is responsible for the different behavior in electrical characteristics after gamma-ray interactions.

36 MATERIALS SCIENCE↗

Titanium-Water Thermosyphon Gamma Radiation Exposure and Results

Titanium-water thermosyphons are being considered for use in heat rejection systems for fission power systems. Their proximity to the nuclear reactor will result in some gamma irradiation. Noncondensable gas formation from radiation-induced breakdown of water over time may render portions of the thermosyphon condenser inoperable. A series of developmental thermosyphons were operated at nominal operating temperature under accelerated gamma irradiation, with exposures on the same order of magnitude as that expected in 8 years of heat rejection system operation. Temperature data were obtained during exposure at three locations on each thermosyphon: evaporator, condenser, and condenser end cap. Some noncondensable gas was evident; however, thermosyphon performance was not affected because the noncondensable gas was compressed into the fill tube region at the top of the thermosyphon, away from the heat rejecting fin. The trend appeared to be an increasing amount of noncondensable gas formation with increasing gamma irradiation dose. Hydrogen is thought to be the most likely candidate for the noncondensable gas and hydrogen is known to diffuse through grain boundaries. Post-exposure evaluation of one thermosyphon in a vacuum chamber and at temperature revealed that the noncondensable gas diffused out of the thermosyphon over a relatively short period of time. Further research shows a number of experimental and theoretical examples of radiolysis occurring through gamma radiation alone in pure water.

Sanzi, James, L.A↗

Titanium-Water Thermosyphon Gamma Radiation Effects and Results

Titanium-water thermosyphons are being considered for use in heat rejection systems for fission power systems. Their proximity to the nuclear reactor will result in some exposure to gamma irradiation. Non-condensable gas formation from radiation may breakdown water over time and render a portion of the thermosyphon condenser inoperable. A series of developmental thermosyphons were operated at nominal operating temperature with accelerated gamma irradiation exposures on the same order of magnitude that is expected in eight years of heat rejection system operation. Temperature data were obtained during exposure at three locations on each thermosyphon; evaporator, condenser, and condenser end cap. Some non-condensable gas was evident, however thermosyphon performance was not affected because the non-condensable gas was compressed into the fill tube region at the top of the thermosyphon, away from the heat rejecting fin. The trend appeared to be an increasing amount of non-condensable gas formation with increasing gamma irradiation dose. Hydrogen is thought to be the most likely candidate for the non-condensable gas and hydrogen is known to diffuse through grain boundaries. Post-exposure evaluation of selected thermosyphons at temperature and in a vacuum chamber revealed that the non-condensable gas likely diffused out of the thermosyphons over a relatively short period of time. Further research shows a number of experimental and theoretical examples of radiolysis occurring through gamma radiation alone in pure water.

Sanzi, James L.↗

A Comparison of Radiation-Induced and High-Field Electrically Stress-Induced Interface Defects in Si/SiO 2 MOSFETs via Electrically Detected Magnetic Resonance

Here, we utilize electrically detected magnetic resonance (EDMR) measurements to compare high-field stressed, and gamma irradiated Si/SiO 2 metal–oxide–silicon (MOS) structures. We utilize spin-dependent recombination (SDR) EDMR detected using the Fitzgerald and Grove dc I-V approach to compare the effects of high-field electrical stressing and gamma irradiation on defect formation at and near the Si/SiO 2 interface. As anticipated, both greatly increase the concentration of P b centers (silicon dangling bonds at the interface) densities. The irradiation also generated a significant increase in the dc I-V EDMR response of E' centers (oxygen vacancies in the SiO 2 films), whereas the generation of an E' EDMR response in high-field stressing is much weaker than in the gamma irradiation case. These results likely suggest a difference in their physical distribution resulting from radiation damage and high electric field stressing.

42 ENGINEERING↗

Milestone 1.2.11: H 2 Production from Surrogate Non-Native Corrosion Plumes on Aluminum 6061-T6 Fuel Cladding Surrogates

Thick, localized, “non-native” corrosion plumes have been identified on Advanced Test Reactor fuel elements, raising concern on their impact on the radiolytic formation of molecular hydrogen gas (H 2 ) from aluminum-clad spent nuclear fuel (ASNF) under proposed extended (> 50 years) dry storage conditions. Here, we report our findings on H 2 generation from the gamma irradiation (up to 52 MGy) of surrogate “non-native” corrosion plume coupons: ambient-temperature-corroded (~350 days in water) aluminum alloy 6061 (AA6061) coupons in helium gas environments with ~0% added relative humidity. Additionally, we provide a comparison of proposed ASNF drying techniques— vacuum drying only, vacuum drying + 100 °C for 4 hr, and vacuum drying + 220 °C for 4 hr—on the yield of H 2 from these surrogate systems. The presented data indicates that similar amounts of H 2 (~2 × 10–3 µmol J–1) are formed from gamma irradiated AA6061 coupons corroded under different temperature regimes, i.e., ambient/350 days vs. 90 C/30 days. These findings validate current, complimentary modelling predictions based on high-temperature-corrosion irradiation data only. Further, the application of a heat treatment procedure (100 and 220 °C), in conjunction with vacuum drying, accelerated the rate at which a steady-state H 2 yield was attained, in comparison to vacuum only, due to the removal of H 2 precursors in the form of adsorbed waters. Interestingly, within the confidence limits of our measurements, negligible difference in total H 2 yield was found between the two investigated heat treatment procedures.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

The effect of gamma ray irradiation on few layered MoSe2: A material for nuclear and space applications

In recent years, emerging two-dimensional (2D) materials, such as molybdenum diselenide (MoSe2), have been at the center of attention for many researchers. This is due to their unique and fascinating physicochemical properties that make them attractive in space and defense applications that include shielding harsh irradiation environments. In this study, we examined the effects of gamma (γ) rays at various doses on the structural, chemical, and optical properties of MoSe2 layers. After the samples were exposed to intense gamma radiation (from a 60Co source) with various exposure times to vary the total accumulated dosage (up to 100 kGy), Raman and photoluminescence spectroscopies were used to study and probe radiation-induced changes to the samples. When compared to pristine materials, very few changes in optical properties were typically observed, indicating good robustness with little sensitivity, even at relatively high doses of gamma radiation. The imaging using scanning electron microscopy revealed a number of nano-hillocks that were connected to substrate alterations. X-ray photoelectron spectroscopies revealed that Mo’s binding energies remained the same, but Se’s binding energies blueshifted. We associated this shift with the decrease in Se vacancies that occurred after irradiation as a result of Mo atoms creating adatoms next to Se atoms. When compared to pristine materials, very few changes in optical, chemical, and structural properties were typically observed. These findings highlight the inherent resilience of MoSe2 in hostile radioactive conditions, which spurs additional research into their optical, electrical, and structural characteristics as well as exploration for potential space, energy, and defense applications.

Materials Science↗

Identification and time evolution of thionyl chloride (SOCl 2 ) radiolysis products

In this study, innovative solutions are needed to reduce the amount of high-level waste generated by used nuclear fuel recycling strategies to support the widespread adoption of sustainable nuclear fission energy technologies. To this end, a new sulfur chloride-based process has been developed to recycle zirconium alloy-based materials, which make up a significant fraction of high-level radioactive waste. To support the continued development of this process, we present new data on the potential reaction pathways over time of the products arising from the gamma and electron beam radiolysis of neat thionyl chloride (SOCl 2 ). Interrogation of the gamma irradiated liquid by Raman spectroscopy provided more conclusive identification of the SOCl 2 degradation products, specifically sulfur dichloride (SCl 2 ), molecular chlorine (Cl 2 ), sulfur dioxide (SO 2 ), and sulfuryl chloride (SO 2 Cl 2 ). In comparison, the high dose rate (~10 7 Gy s -1 ) electron beam irradiations formed significantly more degradation products. For both cobalt-60 gamma and electron beam irradiations, the observed degradation products were found to evolve as a function of time post-irradiation via the same reaction pathways, with indication of a solvent regeneration mechanism. These findings are fortuitous for process development, as such a mechanism would be beneficial for process longevity and cost effectiveness.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Why ionizing radiation enhances surface wettability

Radiation-Induced Surface Activation is an inherent phenomenon where surfaces that are exposed to gamma irradiation are observed to undergo an increase in wettability. This increase in wettability as a result of the ionizing radiation exposure has so far been demonstrated to have a pronounced impact on Leidenfrost temperature and two-phase fluid dynamics. Test results from previous experiments have shown that incorporation of this effect on heat transfer equipment design may increase the thermal-hydraulic margin leading to higher thermal efficiency. However, the mechanism behind the increased wettability is not clearly understood. In the present work, three different materials (Zircaloy-4, 316 stainless steel, and copper) were exposed at two different dose rates with use of two different gamma irradiation facilities. A detailed surface characterization on the post-irradiated samples is carried out to understand the changes in surface chemistry, wettability and surface morphology. It is observed from the experiments that the increase in wettability upon irradiation depended on the total dose and not on the dose rate. Moreover, localized oxidation and porosity induced by radiolysis was seen to be the predominant mechanism behind increased wettability which leads to improved Leidenfrost temperature.

36 MATERIALS SCIENCE↗