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At least 235 records · Page 13

Structural Features of Zirconium-Based Metal–Organic Frameworks Affecting Radiolytic Stability

Metal–organic frameworks (MOFs) NU-1000 and UiO-66 are herein exposed to two different gamma irradiation doses and dose rates and analyzed to determine the structural features that affect their stability in these environments. MOFs have shown promise for the capture and sensing of off-gases at civilian nuclear energy reprocessing sites, nuclear waste repositories, and nuclear accident locations. However, little is understood about the structural features of MOFs that contribute to their stability levels under the ionizing radiation conditions present at such sites. This study is the first of its kind to explore the structural features of MOFs that contribute to their radiolytic stability. Both NU-1000 and UiO-66 are MOFs that contain Zr metal-centers with the same metal absorption cross section. However, the two MOFs exhibit different linker connectivities, linker aromaticities, node densities, node connectivities, and interligand separations. In this study, NU-1000 and UiO-66 were exposed to high (423.3 Gy/min, 23 min, and 37 s) and low (0.78 Gy/min, 4320 min) dose rates of 60 Co gamma irradiation. NU-1000 displayed insignificant radiation damage under both dose rates due to its high linker connectivity, low node density, and low node connectivity. However, low radiation dose rates caused considerable damage to UiO-66, a framework with lower aromaticity and smaller interligand separation. Finally, results suggest that chronic, low-radiation environments are more detrimental to Zr MOF stability than acute, high-radiation conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of Nd(II) and Nd(III) Ions on the Speciation and Kinetic Dynamics of Radiolytic Transients in Molten LiCl-KCl Eutectic Salt Mixtures

In the pyrochemical reprocessing of used nuclear fuel, understanding the effects of ionizing radiation on the chemical behavior of fission products in molten chloride eutectic salt is crucial. Here, this study investigates the impact of radiation on the chemical and kinetic speciation of Nd ions in molten LiCl-KCl eutectic, which are challenging to separate due to their multivalent oxidation states and comproportionation reactions. Electron pulse radiolysis techniques were used to determine transient absorption spectra, chemical kinetics, and activation parameters for the reaction of Nd ions with the primary products of molten LiCl-KCl eutectic radiolysis: the solvated electron (e S - ) and dichlorine radical anion (Cl 2 •- ). Initially, Nd(III) reacted rapidly with e S - , forming Nd(II) with a second-order rate coefficient of k = (4.54 ± 0.07) × 10 10 M -1 s -1 at 673 K. The resulting Nd(II) ions then reacted slowly with Cl 2 •- , regenerating Nd(III) with an estimated rate of k = (1.72 ± 0.04) × 10 10 M -1 s -1 at 673 K. Additionally, the comproportionation reaction of Nd(III) and Nd(s) to form Nd(II) was monitored chemically and electrochemically. This work suggests that the comproportionation reaction of Nd(III) with Nd(s) to form Nd(II) is unstable in molten LiCl-KCl eutectic.

36 - MATERIALS SCIENCE↗

Direct Observation of Morphological and Chemical Changes during the Oxidation of Model Inorganic Ligand-Capped Particles

Functionalization and volatilization are competing reactions during the oxidation of carbonaceous materials and are important processes in many different areas of science and technology. Here, we present a combined ambient pressure X-ray photoelectron spectroscopy (APXPS) and grazing incidence X-ray scattering (GIXS) investigation of the oxidation of oleic acid ligands surrounding NaYF 4 nanoparticles (NPs) deposited onto SiO x /Si substrates. While APXPS monitors the evolution of the oxidation products, GIXS provides insight into the morphology of the ligands and particles before and after the oxidation. Our investigation shows that the oxidation of the oleic acid ligands proceeds at O 2 partial pressures of below 1 mbar in the presence of X-rays, with the oxidation eventually reaching a steady state in which mainly CH x and –COOH functional groups are observed. The scattering data reveal that the oxidation and volatilization reaction proceeds preferentially on the side of the particle facing the gas phase, leading to the formation of a chemically and morphologically asymmetric ligand layer. This comprehensive picture of the oxidation process could be obtained only by combining the X-ray scattering and APXPS data. The investigation presented here lays the foundation for further studies of the stability of NP layers in the presence of reactive trace gases and ionizing radiation and for other nanoscale systems where chemical and morphological changes happen simultaneously and cannot be understood in isolation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Proton irradiation-decelerated intergranular corrosion of Ni-Cr alloys in molten salt

The effects of ionizing radiation on materials often reduce to "bad news". Radiation damage usually leads to detrimental effects such as embrittlement, accelerated creep, phase instability, and radiation-altered corrosion. Here we report that proton irradiation decelerates intergranular corrosion of Ni-Cr alloys in molten fluoride salt at 650 °C. We demonstrate this by showing that the depth of intergranular voids resulting from Cr leaching into the salt is reduced by proton irradiation alone. Interstitial defects generated from irradiation enhance diffusion, more rapidly replenishing corrosion-injected vacancies with alloy constituents, thus playing the crucial role in decelerating corrosion. Our results show that irradiation can have a positive impact on materials performance, challenging our view that radiation damage usually results in negative effects.

36 MATERIALS SCIENCE↗

Bright and durable scintillation from colloidal quantum shells

Abstract Efficient, fast, and robust scintillators for ionizing radiation detection are crucial in various fields, including medical diagnostics, defense, and particle physics. However, traditional scintillator technologies face challenges in simultaneously achieving optimal performance and high-speed operation. Herein we introduce colloidal quantum shell heterostructures as X-ray and electron scintillators, combining efficiency, speed, and durability. Quantum shells exhibit light yields up to 70,000 photons MeV −1 at room temperature, enabled by their high multiexciton radiative efficiency thanks to long Auger-Meitner lifetimes (>10 ns). Radioluminescence is fast, with lifetimes of 2.5 ns and sub-100 ps rise times. Additionally, quantum shells do not exhibit afterglow and maintain stable scintillation even under high X-ray doses (>10 9 Gy). Furthermore, we showcase quantum shells for X-ray imaging achieving a spatial resolution as high as 28 line pairs per millimeter. Overall, efficient, fast, and durable scintillation make quantum shells appealing in applications ranging from ultrafast radiation detection to high-resolution imaging.

47 OTHER INSTRUMENTATION↗

Synchronous detection of cosmic rays and correlated errors in superconducting qubit arrays

Quantum information processing at scale will require sufficiently stable and long-lived qubits, likely enabled by error-correction codes. Several recent superconducting-qubit experiments, however, reported observing intermittent spatiotemporally correlated errors that would be problematic for conventional codes, with ionizing radiation being a likely cause. Here, we directly measured the cosmic-ray contribution to spatiotemporally correlated qubit errors. We accomplished this by synchronously monitoring cosmic-ray detectors and qubit energy-relaxation dynamics of 10 transmon qubits distributed across a 5 × 5 × 0.35 mm 3 silicon chip. Cosmic rays caused correlated errors at a rate of $1/\left(592\begin{array}{c}+48\\ -41\end{array}\,{\rm{s}}\right)$, accounting for 17.1 ± 1.3% of all such events. Our qubits responded to essentially all of the cosmic rays and their secondary particles incident on the chip, consistent with the independently measured arrival flux. Moreover, we observed that the landscape of the superconducting gap in proximity to the Josephson junctions dramatically impacts the qubit response to cosmic rays. Given the practical difficulties associated with shielding cosmic rays, our results indicate the importance of radiation hardening—for example, superconducting gap engineering—to the realization of robust quantum error correction.

Science & Technology - Other Topics↗

CsPbBr3 perovskite detectors with 1.4% energy resolution for high-energy γ-rays

Halide perovskite semiconductors are poised to revitalize the field of ionizing radiation detection as they have done to solar photovoltaics. We show that all-inorganic perovskite CsPbBr 3 devices resolve 137 Cs 662-keV γ-rays with 1.4% energy resolution, as well as other X- and γ-rays with energies ranging from tens of keV to over 1 MeV in ambipolar sensing and unipolar hole-only sensing modes with crystal volumes of 6.65 mm 3 and 297 mm 3 , respectively. Furthermore, we report the scale-up of CsPbBr 3 ingots to up to 1.5 inches in diameter with an excellent hole mobility–lifetime product of 8 × 10 -3 cm 2 V -1 and a long hole lifetime of up to 296 μs. CsPbBr 3 detectors demonstrate a wide temperature region from ~2 °C to ~70 °C for stable operation. Detectors protected with suitable encapsulants show a uniform response for over 18 months. Consequently, we identify perovskite CsPbBr 3 semiconductor as an exceptional candidate for new-generation high-energy γ-ray detection.

47 OTHER INSTRUMENTATION↗

Search for Majorana neutrinos exploiting millikelvin cryogenics with CUORE

The possibility that neutrinos may be their own antiparticles, unique among the known fundamental particles, arises from the symmetric theory of fermions proposed by Ettore Majorana in 1937. Given the profound consequences of such Majorana neutrinos, among which is a potential explanation for the matter–antimatter asymmetry of the universe via leptogenesis, the Majorana nature of neutrinos commands intense experimental scrutiny globally; one of the primary experimental probes is neutrinoless double beta (0νββ) decay. Here we show results from the search for 0νββ decay of 130 Te, using the latest advanced cryogenic calorimeters with the CUORE experiment3. CUORE, operating just 10 millikelvin above absolute zero, has pushed the state of the art on three frontiers: the sheer mass held at such ultralow temperatures, operational longevity, and the low levels of ionizing radiation emanating from the cryogenic infrastructure. We find no evidence for 0νββ decay and set a lower bound of the process half-life as 2.2 × 10 25 years at a 90 percent credibility interval. We discuss potential applications of the advances made with CUORE to other fields such as direct dark matter, neutrino and nuclear physics searches and large-scale quantum computing, which can benefit from sustained operation of large payloads in a low-radioactivity, ultralow-temperature cryogenic environment.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Advanced antireflection for back-illuminated silicon photomultipliers to detect faint light

Silicon photomultipliers have attracted increasing attention for detecting low-density light in both scientific research and practical applications in recent years; yet the photon losses due to reflection on the light-sensitive planar silicon surface considerably limit its photon detection efficiency. Here we demonstrate an advanced light trapping feature by developing the multi-layer antireflection coatings and the textured silicon surface with upright random nano-micro pyramids, which significantly reduces the reflection of faint light in a wide spectrum, from ultraviolet to infrared. Integrating this advanced photon confinement feature into next-generation back-illuminated silicon photomultiplier would increase the photon detection efficiency with significantly lower reflection and much more active areas. This advanced design feature offers the back-illuminated silicon photomultiplier broader application opportunities exemplified in the emerging scenarios such as nuclear medical imaging, light detection and ranging for autonomous driving, detection of scintillation light in ionizing radiation, as well as high energy physics.

42 ENGINEERING↗

Low dose rate γ-irradiation protects fruit fly chromosomes from double strand breaks and telomere fusions by reducing the esi-RNA biogenesis factor Loquacious

Abstract It is still continuously debated whether the low-dose/dose-rate (LDR) of ionizing radiation represents a hazard for humans. Model organisms, such as fruit flies, are considered valuable systems to reveal insights into this issue. We found that, in wild-type Drosophila melanogaster larval neuroblasts, the frequency of Chromosome Breaks (CBs), induced by acute γ-irradiation, is considerably reduced when flies are previously exposed to a protracted dose of 0.4 Gy delivered at a dose rate of 2.5 mGy/h. This indicates that this exposure, which is associated with an increased expression of DNA damage response proteins, induces a radioadaptive response (RAR) that protects Drosophila from extensive DNA damage. Interestingly, the same exposure reduces the frequency of telomere fusions (TFs) from Drosophila telomere capping mutants suggesting that the LDR can generally promote a protective response on chromatin sites that are recognized as DNA breaks. Deep RNA sequencing revealed that RAR is associated with a reduced expression of Loquacious D (Loqs-RD) gene that encodes a well-conserved dsRNA binding protein required for esiRNAs biogenesis. Remarkably, loss of Loqs mimics the LDR-mediated chromosome protection as it decreases the IR-induced CBs and TFs frequency. Thus, our molecular characterization of RAR identifies Loqs as a key factor in the cellular response to LDR and in the epigenetic routes involved in radioresistance.

Porrazzo, A.↗

Impact of iodide ions on the speciation of radiolytic transients in molten LiCl–KCl eutectic salt mixtures

The fate of fission-product iodine is critical for the deployment of next generation molten salt reactor technologies, owing to its volatility and biological impacts if it were to be released into the environment. To date, little is known on how ionizing radiation fields influence the redox chemistry, speciation, and transport of iodine in high temperature molten salts. Here we employ picosecond electron pulse irradiation techniques to elucidate for the first time the impact of iodide ions (I – ) on the speciation and chemical kinetics of the primary radiation-induced transient radicals generated in molten chloride salt mixtures (e S – and Cl 2 ˙– ) as a function of temperature (400–700 °C). In the presence of I – ions (≥ 1 wt% KI in LiCl–KCl eutectic), we find that the transient spectrum following the electron pulse is composed of at least three overlapping species: the e S – and the Cl 2 ˙– and ICl ˙– radical anions, for which a deconvoluted spectrum of the latter is reported here for the first time in molten salts. This new transient spectrum was consistent with gas phase density functional theory calculations. The lifetime of the e S – was unaffected by the addition of I – ions. The newly observed interhalogen radical anion, ICl˙ – , exhibited a lifetime on the order of microseconds over the investigated temperature range. The associated chemical kinetics indicate that the predominate mechanism of ICl˙ – decay is via reaction with the Cl 2 ˙– radical anion. The iodine containing product of this reaction is expected to be ICl 2 – , which will have implications for the transport of fission-product iodine in MSR technologies.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Spectral analysis and kinetic modeling of radioluminescence in air and nitrogen

Here, in this article we present a quantitative analysis of the second positive system of molecular nitrogen and the first negative system of the molecular nitrogen cation excited in the presence of ionizing radiation. Optical emission spectra of atmospheric air and nitrogen surrounding 210 Po sources were measured from 250 to 400 nm. Multi-Boltzmann and non-Boltzmann vibrational distribution spectral models were used to determine the vibrational temperature and vibrational distribution function of the emitting N 2 (C 3 Π u ) and N 2 + (B 2 Σ + u ) states. A zero-dimensional kinetic model, based on the electron energy distribution function (EEDF) and steady-state excitation and de-excitation of N 2 (X 1 Σ + g ), N 2 + (B 2 Σ + u ), N 2 + (X 2 Σ + g ), N 4 + , O 2 + , and N 2 (C 3 Π u , v), was developed for the prediction of the relative spectral intensity of both the N 2 + (B 2 Σ + u → X 2 Σ + g ) emission band and the vibrational bands of N 2 (C 3 Π u → B 3 Π g ) for comparison with the experimental data.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Structural and physical properties of two distinct 2D lead halides with intercalated Cu( II )

Transition metal cation intercalation between the layers of two-dimensional (2D) metal halides is an underexplored research area. In this work we focus on the synthesis and physical property characterizations of two layered hybrid lead halides: a new compound [Cu(O 2 C–CH 2 –NH 2 ) 2 ]Pb 2 Br 4 and the previously reported [Cu(O 2 C–(CH 2 ) 3 –NH 3 ) 2 ]PbBr 4 . These compounds exhibit 2D layered crystal structures with incorporated Cu 2+ between the metal halide layers, which is achieved by combining Cu(II) and lead bromide with suitable amino acid precursors. The resultant [Cu(O 2 C–(CH 2 ) 3 –NH 3 ) 2 ]PbBr 4 adopts a 2D layered perovskite structure, whereas the new compound [Cu(O 2 C–CH 2 –NH 2 ) 2 ]Pb 2 Br 4 crystallizes with a new structure type based on edge-sharing dodecahedral PbBr5O3 building blocks. [Cu(O 2 C–CH 2 –NH 2 ) 2 ]Pb 2 Br 4 is a semiconductor with a bandgap of 3.25 eV. It shows anisotropic charge transport properties with a semiconductor resistivity of 1.44 × 10 10 Ω cm (measured along the a-axis) and 2.17 × 10 10 Ω cm (along the bc-plane), respectively. The fabricated prototype detector based on this material showed response to soft low-energy X-rays at 8 keV with a detector sensitivity of 1462.7 μCGy –1 cm –2 , indicating its potential application for ionizing radiation detection. Finally, these encouraging results are discussed together with the results from density functional theory calculations, optical, magnetic, and thermal property characterization experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

First demonstration of a fiber optic bolometer on a tokamak plasma (invited)

A fiber optic bolometer (FOB) was demonstrated observing a fusion plasma for the first time at the DIII-D tokamak. A FOB uses a fiber optics-based interferometric technique that is designed to have a high sensitivity to temperature changes [75 mK/(W/m2) responsivity in high vacuum with 0.38 mK noise level] with a negligible susceptibility to electromagnetic interference (EMI) that can be problematic for resistive bolometers in a tokamak environment. A single-channel test apparatus was installed on DIII-D consisting of a measurement FOB and shielded reference FOB. The single-channel FOB showed a negligible increase in the noise level during typical plasma operations (0.39 mK) compared to the benchtop results (0.38 mK), confirming an insignificant EMI impact to the FOB. Comparisons to DIII-D resistive bolometers showed good agreement with the single-channel FOB, indicating that the FOB is comparable to a resistive bolometer when the impulse calibration is applied. The noise-equivalent power density of the calibrated FOB during a plasma operation was 0.55 W/m2 with an average sampling time of 20 ms. The major potential effect of ionizing radiation on the FOB would be the radiation-induced attenuation, which can be efficiently compensated for by adjusting the probing light power.

Lee, S. (ORCID:0000000170289004)↗

Scintillation of colloidal nanocrystals

Scintillators are materials that convert ionizing radiation in the form of particles or photons into low-energy photons in the ultraviolet to near-infrared spectral range. Here, this work reviews efforts to use colloidal nanocrystals as scintillator materials. To date, research on colloidal nanocrystals as scintillators has focused on doped phosphor systems, quantum dots and related structures, and perovskite-based nanocrystals. Among various material classes and forms, colloidal semiconductor nanocrystals stand out thanks to their appealing fluorescence properties, yet understanding of their radioluminescence and cathodoluminescence is incomplete. This review discusses fundamental limits and material design challenges toward achieving high brightness, fast speed, and durable scintillator performance with nanocrystal scintillators. First, this review describes the basic principles and efficiency limitations of scintillation, particularly the large influence of multiple exciton generation in many nanocrystal species, as well as performance metrics. Second, methods for measurement are described. Third, we review the results of the main classes of nanocrystal scintillators, including quantum dots and related particles, perovskites, and doped-phosphor particles. Fourth, scintillation imaging is discussed in terms of the relevant performance metrics and results obtained using nanocrystal materials. Finally, we note the strengths and weaknesses of nanocrystal scintillators and discuss potential areas of further development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mortality among Tennessee Eastman Corporation (TEC) uranium processing workers, 1943–2019

Background: There are few occupational studies of women exposed to ionizing radiation. During World War II, the Tennessee Eastman Corporation (TEC) operated an electromagnetic field separation facility of 1152 calutrons to obtain enriched uranium (235U) used for the Hiroshima atomic bomb. Thousands of women were involved in these operations. Materials and methods: We report a new study was conducted of 13,951 women and 12,699 men employed at TEC between 1943 and 1947 for at least 90 days. Comprehensive dose reconstruction techniques were used to estimate lung doses from the inhalation of uranium dust based on airborne measurements. Vital status through 2018/2019 was obtained from the National Death Index, Social Security Death Index, Tennessee death records and online public record databases. Analyses included standardized mortality ratios (SMRs) and Cox proportional hazards models. Results: Most workers were hourly (77.7%), white (95.6%), born before 1920 (58.3%), worked in dusty environments (57.0%), and had died (94.9%). Vital status was confirmed for 97.4% of the workers. Women were younger than men when first employed: mean ages 25.0 years and 33.0 years, respectively. The estimated mean absorbed dose to the lung was 32.7 mGy (max 1048 mGy) for women and 18.9 mGy (max 501 mGy) for men. The mean dose to thoracic lymph nodes (TLNs) was 127 mGy. Statistically significant SMRs were observed for lung cancer (SMR 1.25; 95% CI 1.19, 1.31; n = 1654), nonmalignant respiratory diseases (NMRDs) (1.23; 95% CI 1.19, 1.28; n = 2585), and cerebrovascular disease (CeVD) (1.13; 95% CI 1.08, 1.18; n = 1945). For lung cancer, the excess relative rate (ERR) at 100 mGy (95% CI) was 0.01 (–0.10, 0.12; n = 652) among women, and –0.15 (–0.38, 0.07; n = 1002) among men based on a preferred model for men with lung doses <300 mGy. NMRD and non-Hodgkin lymphoma were not associated with estimated absorbed dose to the lung or TLN. Conclusions: There was little evidence that radiation increased the risk of lung cancer, suggesting that inhalation of uranium dust and the associated high-LET alpha particle exposure to lung tissue experienced over a few years is less effective in causing lung cancer than other types of exposures. There was no statistically significant difference in the lung cancer risk estimates between men and women. The elevation of certain causes of death such as CeVD is unexplained and will require additional scrutiny of workplace or lifestyle factors given that radiation is an unlikely contributor since only the lung and lymph nodes received appreciable dose.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Conceptual study of a two-layer silicon pixel detector to tag the passage of muons from cosmic sources through quantum processors

Abstract Recent studies in quantum computing have shown that quantum error correction with large numbers of physical qubits are limited by ionizing radiation from high-energy particles. Depending on the physical setup of the quantum processor, the contribution of muons from cosmic sources can constitute a significant fraction of these interactions. As most of these muons are difficult to stop, we perform a conceptual study of a two-layer silicon pixel detector to tag their hits on a solid-state quantum processor instead. With a typical dilution refrigerator geometry model, we find that efficiencies greater than 50% are most likely to be achieved if at least one of the layers is operated at the deep-cryogenic (<1 K) flanges of the refrigerator. Following this finding, we further propose a novel research program that could allow the development of silicon pixel detectors that are fast enough to provide input to quantum error correction algorithms, can operate at deep-cryogenic temperatures, and have very low power consumption.

Instruments & Instrumentation↗

Design of the cryogenic moderator system for the second target station

The Second Target Station (STS) at Oak Ridge National Laboratory will be a 700 kW pulsed spallation neutron source designed to provide the world's highest brightness cold neutron beams. In order to produce the required neutron performance, two compact liquid hydrogen moderators are located adjacent to the tungsten spallation target and must be supplied with less than 20 K hydrogen and a para hydrogen fraction of 99.8% or greater. The Cryogenic Moderator System (CMS) will consist of a single hydrogen loop feeding the two moderators in series cooled by a helium refrigerator with a cooling capacity of 2.5 kW at 17 K. The hydrogen loop consists of a hydrogen circulator, hydrogen helium heat exchanger, ortho-para converter, accumulator, transfer lines and heater. The design of the hydrogen loop is based on the CMS design of the First Target Station at the Spallation Neutron Source and some of the component designs may be reused. General hydrogen temperature control is provided by controlling the flowrate of helium to the heat exchanger. The hydrogen loop will have a constant flowrate of 0.5 L/s and remove a nuclear heat load of about 850 W from the two moderators, which is deposited both directly in the hydrogen and the adjacent hydrogen containing structures. Because the nuclear heat load is accelerator driven, the hydrogen system must remain stable when the heat load is removed instantaneously during beam trips. System stability is maintained passively with the accumulator and actively with the heater. Ionizing radiation which interacts with the liquid hydrogen drives backconversion of the hydrogen from parahydrogen to orthohydrogen. The STS moderator performance is very sensitive to small fractions of orthohydrogen requiring an ortho-para converter to maintain the hydrogen supplied to the moderators at near equilibrium parahydrogen concentration. STS CMS is in the early stage of preliminary design and current focus is evaluating component sizing and system stability during beam transients.

Janney, Jim↗