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At least 793 records · Page 44

Formation of ion damage tracks

A new model is proposed to explain both localized damage regions and preferential etching of damage tracks caused by the passage of energetic ions in insulators. The formation of each region of extended defects is initiated by the Auger decay of a vacancy produced in an inner electronic shell of an atom of the insulator by an incident ion. This decay produces an intense source of ionization within a small volume around the decaying atom, which causes decomposition of the material in a manner similar to that observed in pulsed laser irradiation. The resulting chemical or crystalline modification of the material is the latent track, which can be preferentially etched due to its changed structure.

Tombrello, T. A.↗

Quantifying Low Energy Proton Damage in Multijunction Solar Cells

An analysis of the effects of low energy proton irradiation on the electrical performance of triple junction (3J) InGaP2/GaAs/Ge solar cells is presented. The Monte Carlo ion transport code (SRIM) is used to simulate the damage profile induced in a 3J solar cell under the conditions of typical ground testing and that of the space environment. The results are used to present a quantitative analysis of the defect, and hence damage, distribution induced in the cell active region by the different radiation conditions. The modelling results show that, in the space environment, the solar cell will experience a uniform damage distribution through the active region of the cell. Through an application of the displacement damage dose analysis methodology, the implications of this result on mission performance predictions are investigated.

Messenger, Scott R.↗

Radiation‐Induced Defects in Uranyl Trinitrate Solids

Abstract Actinides are inherently radioactive; thus, ionizing radiation is emitted by these elements can have profound effects on its surrounding chemical environment through the formation of free radical species. While previous work has noted that the presence of free radicals in the system impacts the redox state of the actinides, there is little atomistic understanding of how these metal cations interact with free radicals. Herein, we explore the effects of radiation (UV and γ) on three U(VI) trinitrate complexes, M[UO 2 (NO 3 ) 3 ] (where M=K + , Rb + , Cs + ), and their respective nitrate salts in the solid state via electron paramagnetic resonance (EPR) and Raman spectroscopy paired with Density Functional Theory (DFT) methods. We find that the alkali salts form nitrate radicals under UV and γ irradiation, but also note the presence of additional degradation products. M[UO 2 (NO 3 ) 3 ] solids also form nitrate radicals and additional DFT calculations indicate the species corresponds to a change from the bidentate bound nitrate anion into a monodentate NO 3 • radical. Computational studies also highlight the need to include the second sphere coordination environment around the [UO 2 (NO 3 ) 3 ] 0,1 species to gain agreement between the experimental and predicted EPR signatures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Scanning Transmission Electron Microscopy–Atom Probe Tomography Correlative Analysis for the Characterization of Solute-defect Interactions

Atom probe tomography (APT) and (scanning) transmission electron microscopy ((S)TEM) are complementary techniques that provide spatially resolved chemical and structural information at the atomic scale. Here, in this study, we employ two different STEM/APT correlative analysis methods to investigate Cr segregation at dislocation loops in ultra-high purity Fe–Cr alloys. APT needles for the correlative analysis were extracted either from bulk material or from thinned TEM lamellae. STEM analysis was used to determine the Burgers vectors of ion-irradiation-induced dislocation loops, while APT reconstruction of the same region revealed the Cr segregation to these loops. We extended the g•b = 0 invisibility criterion of dislocation loops from TEM mode in a lamella to STEM mode in a needle-shaped specimen. STEM and APT analysis on the same needle provide straightforward correlative analysis, although it is limited by a small observation volume. In contrast, iterative STEM analysis of TEM lamellae, followed by the selective extraction of specific regions of interest for APT analysis, expands the observation area by up to 100 times but requires additional time-consuming steps for APT needle extraction from the lamellae.

47 OTHER INSTRUMENTATION↗

London penetration depth of electron-irradiated Ba 0 . 47 K 0 . 53 Fe 2 As 2

We have characterized an electron-irradiated Ba 1-x K x Fe 2 As 2 (x = 0.53) single-crystal using two different experimental techniques: magneto-optic measurements and microwave measurements. The crystal has been measured before as well as after the 2.5 MeV electron irradiation process. After irradiation it was annealed in a number of steps, between 90 °C and 180 °C, and measured after each annealing step. Most microwave measurements were performed by means of a copper cavity, taking advantage of the TE 011 and TM 110 modes, allowing for the determination of the London penetration depths changes δλ ab (T) and δλ c (T), ie perpendicular and parallel to the sample c-axis. Appropriate equations, based on perturbation theory, were derived to calculate the penetration depths changes δλ ab and δλ c for a rectangular prism geometry. The sample showed a full recovery of its T c , however the observed behavior of δλ c and δλ ab was not monotonic vs annealing temperature, displaying a minimum of δλ c and δλ ab at 120 °C. In conclusion, this finding was confirmed by magneto-optic measurements, where besides verifying the sample uniformity and the absence of visible defects, the lower critical field H c1 of the Ba 1-x K x Fe 2 As 2 single-crystal was obtained and the London penetration depth λab(0) was calculated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Analysis of Chromosomal Aberrations after Low and High Dose Rate Gamma Irradiation in ATM or NBS Suppressed Human Fibroblast Cells

A detailed understanding of the biological effects of heavy nuclei is needed for space radiation protection and for cancer therapy. High-LET radiation produces more complex DNA lesions that may be non-repairable or that may require additional processing steps compared to endogenous DSBs, increasing the possibility of misrepair. Interplay between radiation sensitivity, dose, and radiation quality has not been studied extensively. Previously we studied chromosome aberrations induced by low- and high- LET radiation in several cell lines deficient in ATM (ataxia telangactasia mutated; product of the gene that is mutated in ataxia telangiectasia patients) or NBS (nibrin; product of the gene mutated in the Nijmegen breakage syndrome), and gliomablastoma cells that are proficient or lacking in DNA-dependent protein kinase (DNA-PK) activity. We found that the yields of both simple and complex chromosomal aberrations were significantly increased in the DSB repair defective cells compared to normal cells. The increased aberrations observed for the ATM and NBS defective lines was due to a significantly larger quadratic dose-response term compared to normal fibroblasts for both simple and complex aberrations, while the linear dose-response term was significantly higher in NBS cells only for simple exchanges. These results point to the importance of the functions of ATM and NBS in chromatin modifications that function to facilitate correct DSB repair and minimize aberration formation. To further understand the sensitivity differences that were observed in ATM and NBS deficient cells, in this study, chromosomal aberration analysis was performed in normal lung fibroblast cells treated with KU-55933, a specific ATM kinase inhibitor, or Mirin, an MRN complex inhibitor involved in activation of ATM. We are also testing siRNA knockdown of these proteins. Normal and ATM or NBS suppressed cells were irradiated with gamma-rays and chromosomes were collected with a premature chromosome condensation (PCC) technique at the first mitosis post-irradiation. Chromosomes were analyzed using a multicolor fluorescence in-situ hybridization (mFISH) chromosome painting method. Preliminary analysis showed that chromosomal exchanges were increased in the cells treated with the specific ATM inhibitor. Possible cytogenetic signatures of acute and low dose-rate gamma irradiation in ATM or Nibrin deficient and suppressed cells will be discussed.

Hada, M.↗

Direct Fabrication of Atomically Defined Pores in MXenes Using Feedback-Driven STEM

Controlled fabrication of nanopores in 2D materials offer the means to create robust membranes needed for ion transport and nanofiltration. Techniques for creating nanopores have relied upon either plasma etching or direct irradiation; however, aberration-corrected scanning transmission electron microscopy (STEM) offers the advantage of combining a sub-Å sized electron beam for atomic manipulation along with atomic resolution imaging. Here, for this work, a method for automated nanopore fabrication is utilized with real-time atomic visualization to enhance the mechanistic understanding of beam-induced transformations. Additionally, an electron beam simulation technique, Electron-Beam Simulator (E-BeamSim) is developed to observe the atomic movements and interactions resulting from electron beam irradiation. Using the MXene Ti 3 C 2 T x , the influence of temperature on nanopore fabrication is explored by tracking atomic transformations and find that at room temperature the electron beam irradiation induces random displacement and results in titanium pileups at the nanopore edge, which is confirmed by E-BeamSim. At elevated temperatures, after removal of the surface functional groups and with the increased mobility of atoms results in atomic transformations that lead to the selective removal of atoms layer by layer. This work can lead to the development of defect engineering techniques within functionalized MXene layers and other 2D materials.

36 MATERIALS SCIENCE↗

Radiation Damage and Mitigation by Minority Carrier Injection in InAsSb/AlAsSb Heterojunction Barrier Mid-Wave Infrared Detector

Here, the effects of gamma and proton irradiation, and of forward bias minority carrier injection, on photo-response were investigated for InAsSb/AlAsSb pBn mid-wave infrared (MWIR) detectors with an engineered majority-carrier barrier. Room-temperature gamma irradiation had an insignificant effect on 77 K photo-response. Gamma irradiation at 77 K detector temperature, however, decreased in situ photo-response by 19% after a cumulative dose of ~ 500 krad(Si). Subsequent forward bias minority carrier injection had no effect on photo-response. The 77 K detectors irradiated with 30 MeV protons up to 2 Mrad(Si) had photo-response degraded by up to 70%, but here forward bias minority carrier (hole) injection caused up to 12% recovery that persisted more than 30 min. These results suggest a mitigation strategy for maintaining the photo-response of similar detectors in radiation environments that cause displacement damage defects.

36 MATERIALS SCIENCE↗

The effects of lithium counterdoping on radiation damage and annealing in n(+)p silicon solar cells

Boron-doped silicon n(+)p solar cells were counterdoped with lithium by ion implantation and the resultant n(+)p cells irradiated by 1 MeV electrons. Performance parameters were determined as a function of fluence and a deep level transient spectroscopy (DLTS) study was conducted. The lithium counterdoped cells exhibited significantly increased radiation resistance when compared to boron doped control cells. Isochronal annealing studies of cell performance indicate that significant annealing occurs at 100 C. Isochronal annealing of the deep level defects showed a correlation between a single defect at E sub v + 0.43 eV and the annealing behavior of short circuit current in the counterdoped cells. The annealing behavior was controlled by dissociation and recombination of this defect. The DLTS studies showed that counterdoping with lithium eliminated three deep level defects and resulted in three new defects. The increased radiation resistance of the counterdoped cells is due to the interaction of lithium with oxygen, single vacancies and divacancies. The lithium-oxygen interaction is the most effective in contributing to the increased radiation resistance.

Weinberg, I.↗

Electron Beam Induced Luminescence of SiO2 Optical Coatings

Optical coatings of disordered thin film SiO,/SiO, samples undergoing electron beam bombardment exhibited a cathodoluminescence effect. Measurements were made of the absolute illuminance and emission spectra as functions of incident electron energy (0.2 keV to 30 keV). flux (approx. 0.1 nA/sq cm to > 100 nA/sq cm) and power (<50 nW/sq cm to > 3mW/sq cm) for coatings (approx.60 nm to approx.200 nm thick) on reflective metal substrates over a range of sample temperatures (approx.40 K to approx.400 K) and emission wavelengths (approx.260 nm to approx.5000 nm). Illuminance reached a plateau saturation intensity I(sub sat) approx. 10(exp -4)W/sq cm. scaling as [I(sub mc)/(I + I(sub mc)/I(sub sat)] as incident power I(sub mc) approached I(sub sat). Well below I(sub sat), illuminance scaled linearly with incident power for lower-energy non-penetrating radiation that deposited all of its energy in the dielectric film. At higher incident energies (> 1-5 keV) electrons penetrate the dielectric, depositing only a fraction of their energy in the dielectric film, where deposited energy scales as the ratio of film thickness to penetration range. Since electron range exhibits a peak below approx. 1 keV, the illuminance decreased with increasing energy for penetrating radiation. The temperature dependence of the illuminance. in general, increased with decreasing temperature. Changes in apparent color with temperature were also observed. Four bands in the UV/VIS/NIR range from 300 nm to 1000 nm were observed in spectral measurements; no significant luminescence was detected in a range from approx. 1000 nm to approx. 5000 nm. These different bands either increased or decreased in intensity and shifted slightly in energy with decreasing temperature. Our measurements are explained in terms of simple disordered band theory models based on atomic-scale stochastic transport of electrons in highly disordered insulating materials. The theoretical models provide a fundamental basis for understanding the dependence of cathodoluminescence on irradiation time, incident flux and energy. and sample thickness and temperature. The observed luminescence occurs when an incident high energy electron excites a valence band electron into the conduction band. Following the excitation. a complex series of transitions take place between the extended conduction states and the long-lived localized trapped states (or chromophores) associated with structural or compositional defects in the dielectric materials. Thc transport equations and models of thc spatial and energy distribution of the trapped states below the mobility edge, their occupancy, and transitions provide microscopic scale insights into this macroscopic phenomenon. Our observations and theoretical models are also compared with similar previous room temperature studies of similar SiO2 films.

Dennison, J. R.↗

Time resolved studies of proton irradiated quantum dots

The effects of proton irradiation on carrier dynamics were measured by time-resolved photoluminescence on InGaAs/GaAs quantum dot structures with different dot density and substrate orientation, as well as on InAlAs/AlGaAs quantum dots.

nanotechnology↗

High-Entropy Alloy R&D for Accelerator Beam Window Applications

High-Entropy Alloys are a class of novel material that can offer improved resistance to beam-induced radiation damage and thermal shock. Development of these new alloys to serve as beam windows in multi-megawatt accelerator target applications is ongoing at Fermilab. Currently we are investigating AlCoCrMnTiV alloy systems of 4-6 components for service as beam windows; these compositions are predicted by CALPHAD simulation to have a low density and single-phase BCC crystal structure. The microstructures of these systems are being studied by electron microscopy techniques such as energy dispersive X-ray spectroscopy (EDS) to determine elemental homogeneity and composition, electron backscatter diffraction (EBSD) to quantify grain structure and orientation, and transmission electron microscopy (TEM) to observe defect structures and precipitate formation; nanoindentation is used to probe microstructural mechanical properties. Initial bulk property characterization utilizes differential scanning calorimetry to quantify specific heat capacity (cp), dilatometry to determine the coefficient of thermal expansion (CTE), and time-domain thermoreflectance (TDTR) to measure thermal conductivity (K). A miniature tensile testing apparatus is also being developed to test tensile properties. Post-irradiation examination is currently ongoing for several of these compositions that have been irradiated by low-energy ions to damage levels and at a temperature relevant to beam window applications at future next-generation accelerator facilities. This talk will briefly describe the alloy design and synthesis before going into more depth covering microstructural pre-characterization, and post-irradiation examination results from low-energy ion irradiated specimens. This will be followed by the plans for alloy down selection and future prototypic proton irradiations.

43 PARTICLE ACCELERATORS↗

Degradation and recovery mechanisms in lithium-doped solar cells

Several groups of lithium-doped solar cells have been evaluated under 1-MeV electron irradiation. Many of these groups indicated superior electrical output after irradiation and recovery as compared to similarly irradiated n/p solar cells. The superior cells are those with lithium concentrations of 2 to 5 x 10 to the 14th power atoms per cu cm at the junction. An irradiation of lithium-doped cells with 28-MeV electrons indicated a tenfold advantage of lithium-doped cells over n/p cells. Studies of the changes in the lithium concentration during recovery have shown the amounts of lithium reacting is highly nonlinear in regard to the electron fluence and varies greatly with distance from the junction. The results indicate that precipitation of lithium on radiation defects may be the cause of recovery rather than ion pairing.

Downing, R. G.↗

Ion beam irradiation of ABO4 compounds with the fergusonite, monazite, scheelite, and zircon structures

The effects of irradiation on CaWO4, SrWO4, BaWO4, YVO4, LaVO4, YNbO4, and LaNbO4 were investigated on thin crystals using 1.0 MeV Kr ions at 50-1000 K. All of the ABO4 compounds can be amorphized with calculated damage cross sections (σa = 1/Fc0) in the range of ~0.30-1.09 × 10-14 cm2 ion-1 at zero Kelvin. The analysis of fluence-temperature data returned critical temperatures for amorphization (Tc) of 311 ± 1, 358 ± 90, 325 ± 19, 415 ± 17, 541 ± 6, 636 ± 26, and 1012 ± 1 K, respectively, for the compounds listed above. Compared with previous in situ irradiation of ABO4 orthophosphate samples using 0.8 MeV Kr ions, the Tc values of LaVO4 and YVO4 are higher than those of LaPO4 and YPO4 by 82 K and 124 K, respectively. The Tc values of the three scheelite structures, CaWO4, SrWO4, and BaWO4, indicate that they are the most radiation tolerant compounds under these conditions. The A-B cation anti-site energies, EfAB, determined by DFT range from 2.48 to 10.58 eV and are highly correlated with the A-B cation ionic radius ratio, rA/rB, but are not correlated with Tc across the different structure types, suggesting that the formation and migration energies of Frenkel defects play a more important role in damage recovery in these compounds. We also discuss the role of cation and anion charge/iconicity as determined by DFT. ABO4 compounds with the zircon structure and B = P or V have a distinct advantage over those with B = Si as the damaged regions do not appear to be significantly affected by polymerization of (PO4) 3- or (VO4) 3- groups which might stabilize the amorphous fraction and ultimately lead to phase separation as observed in zircon (ZrSiO4).

amorphization↗

Irradiation-induced formation of G-phase precipitates and M 2 X carbides in self-ion irradiated HT-9

Ferritic-martensitic steels with high chromium content are a promising material group for advanced nuclear systems due to their high temperature strength and good irradiation tolerance. HT-9 is an optimized and often-studied alloy in this group, but additional studies are required on its radiation response under extreme conditions to be experienced in various types of nuclear reactors, especially with respect to phase stability under irradiation. Self-ion irradiation of HT-9 by 5 MeV Fe ions was used to simulate neutron-induced behavior reaching peak doses of 100 and 300 dpa at temperatures ranging from 450 to 550 °C. M 23 C 6 carbides that existed prior to irradiation were found to remain stable under all examined irradiation conditions. As irradiation progressed at 450 and 500 °C, however, formation of spherical-like G-phase precipitates and needle-like M 2 X carbides was observed. G-phase precipitates were found to be enriched in Ni, Si, and Mn, and show no interface segregation, whereas needle-like M 2 X carbides were rich in Cr and Mo and clearly displayed interface segregation of Ni and Si. M 2 X carbide formation is believed to be assisted by vacancies, while G-phase precipitation is thought to be assisted by interstitials. Finally, this difference in defect-mediated formation leads to a difference in distribution with depth. M 2 X carbides are distributed over shallower depths than that of G-phase precipitates, consistent with defect imbalance predictions that consider the influence of the injected interstitial effect.

atom probe tomography↗

Indium Tin-Doped Oxide Interactions with Solvent Radiolysis Products

Transparent conductive oxides (TCOs), such as indium tin-doped oxide (ITO), are ubiquitous as components of electronics and are ideal electrode substrates for catalysis, energy transformation reactions, and energy storage applications. Recently, researchers have recognized their effectiveness as electrode materials for manipulating actinide oxidation states in solution. Despite their popularity as electrode materials, prior studies focused extensively on the direct radiolysis of TCO materials in air and rarely examined these effects within a solution, limiting our fundamental understanding of the interactions between solvent radiolysis products and these substrates in high radiation environments. Here, in this study, we characterize the effects of solvent radiolysis products—arising from the gamma irradiation of water, aqueous nitric acid solutions, and n-dodecane—on the composition, surface speciation, and band structure of ITO thin films on a glass substrate as a function of absorbed dose using UV-visible spectroscopy, scanning electron microscopy, photoelectrochemistry, and X-ray photoelectron spectroscopy. Our work demonstrates that mesoporous thin film electrodes of ITO exposed to gamma radiation in each solvent accumulate defects and exhibit solvent and dose dependent changes to their surface and interfacial properties. These electrodes maintain their electrochemical function and improve their photoelectrochemical performance up to at least 100 kGy of accumulated gamma dose, confirming their utility in solvents exposed to ionizing radiation fields.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Photoluminescence and Raman spectroscopy of wide bandgap semiconductors damaged by deep-UV laser irradiation

The effects of a pulsed, focused, deep-UV (4.66 eV) laser on wide and ultra-wide bandgap semiconductors were investigated with photoluminescence (PL) and Raman spectroscopy. Three semiconductor single crystals were studied: silicon carbide (6H-SiC), gallium nitride (GaN), and gallium oxide (β-Ga 2 O 3 ). Atomic emission lines from neutral Ga or Si were observed during the laser-damage process. For all three semiconductors, PL mapping (3.49 eV laser excitation) of the damaged material revealed visible emission bands in the 2.6–2.8 eV range, attributed to point defects. Raman spectra (2.33 eV excitation) showed a reduction in the Raman peak intensities in the damaged region, along with weak PL bands around 1.9–2.1 eV.

36 MATERIALS SCIENCE↗

Quantum Sensing of Insulator‐to‐Metal Transitions in a Mott Insulator

Nitrogen vacancy (NV) centers, optically active atomic defects in diamond, have attracted tremendous interest for quantum sensing, network, and computing applications due to their excellent quantum coherence and remarkable versatility in a real, ambient environment. Taking advantage of these strengths, this paper reports on NV-based local sensing of the electrically driven insulator-to-metal transition (IMT) in a proximal Mott insulator. The resistive switching properties of both pristine and ion-irradiated VO 2 thin film devices are studied by performing optically detected NV electron spin resonance measurements. These measurements probe the local temperature and magnetic field in electrically biased VO 2 devices, which are in agreement with the global transport measurement results. In pristine devices, the electrically driven IMT proceeds through Joule heating up to the transition temperature while in ion-irradiated devices, the transition occurs nonthermally, well below the transition temperature. Here, the results provide direct evidence for nonthermal electrically induced IMT in a Mott insulator, highlighting the significant opportunities offered by NV quantum sensors in exploring nanoscale thermal and electrical behaviors in Mott materials.

McLaughlin, Nathan J.↗