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  1. High entropy ceramics for applications in extreme environments

    Abstract Compositionally complex materials have demonstrated extraordinary promise for structural robustness in extreme environments. Of these, the most commonly thought of are high entropy alloys, where chemical complexity grants uncommon combinations of hardness, ductility, and thermal resilience. In contrast to these metal–metal bonded systems, the addition of ionic and covalent bonding has led to the discovery of high entropy ceramics (HECs). These materials also possess outstanding structural, thermal, and chemical robustness but with a far greater variety of functional properties which enable access to continuously controllable magnetic, electronic, and optical phenomena. In this experimentally focused perspective, we outline the potentialmore » for HECs in functional applications under extreme environments, where intrinsic stability may provide a new path toward inherently hardened device design. Current works on high entropy carbides, actinide bearing ceramics, and high entropy oxides are reviewed in the areas of radiation, high temperature, and corrosion tolerance where the role of local disorder is shown to create pathways toward self-healing and structural robustness. In this context, new strategies for creating future electronic, magnetic, and optical devices to be operated in harsh environments are outlined.« less
  2. Athermal annealing of pre-existing defects in crystalline silicon

    Systematic investigations of electronic energy loss (Se) effects on pre-existing defects in crystalline silicon (Si) are crucial to provide reliance on the use of ionizing irradiation to anneal pre-existing defects, leading to successful implementation of this technology in the fabrication of Si-based devices. In this regard, the Se effects on nonequilibrium defect evolution in pre-damaged Si single crystals at 300 K has been investigated using intermediate-energy ions (12 MeV O and Si ions) that interact with the pre-damaged surface layers of Si mainly by ionization, except at the end of their range where the nuclear energy loss (Sn) is nomore » longer negligible. Furthermore, under these irradiation conditions, experimental results and molecular dynamics simulations have revealed that pre-existing disorder in Si can be almost fully annealed by subsequent irradiation with intermediate-energy incident ions with Se values as low as 1.5–3.0 keV/nm. Selective annealing of pre-existing defect levels in Si at room temperature can be considered as an effective strategy to mediate the transient enhanced diffusion of dopants in Si. This approach is more desirable than the regular thermal annealing, which is not compatible with the processing requirements that fall below the typical thermal budget.« less
  3. Dynamic substrate reactions during room temperature heavy ion irradiation of CoCrCuFeNi high entropy alloy thin films

    Abstract High entropy alloys (HEAs) are promising materials for various applications including nuclear reactor environments. Thus, understanding their behavior under irradiation and exposure to different environments is important. Here, two sets of near-equiatomic CoCrCuFeNi thin films grown on either SiO 2 /Si or Si substrates were irradiated at room temperature with 11.5 MeV Au ions, providing similar behavior to exposure to inert versus corrosion environments. The film grown on SiO 2 had relatively minimal change up to peak damage levels above 500 dpa, while the film grown on Si began intermixing at the substrate–film interface at peak doses of 0.1 dpa before transformingmore » into a multi-silicide film at higher doses, all at room temperature with minimal thermal diffusion. The primary mechanism is radiation-enhanced diffusion via the inverse Kirkendall and solute drag effects. The results highlight how composition and environmental exposure affect the stability of HEAs under radiation and give insights into controlling these behaviors.« less
  4. Laser Doppler vibrometry for piezoelectric coefficient ($$d_{33}$$) measurements in irradiated aluminum nitride

    Sensors used for experiments in advanced reactors must survive in harsh environments. Few material systems can be used to construct sensors viable for extreme conditions. Aluminum nitride (AlN) is one such material because it has high thermal stability and radiation resistance and sustains good piezoelectric and dielectric properties at high temperatures. In this work, the piezoelectric coefficient $$d_{33}$$ of the AlN single-crystal with thermal and irradiation damage was investigated using an indirect method with a laser Doppler vibrometer (LDV). Surface electrodes were deposited on the AlN samples, and the vibration response of the samples to an applied voltage was monitoredmore » using the LDV as a function of the excitation frequency. The $$d_{33}$$ estimation was based on the excitation voltage and the thickness-mode displacement extracted from the LDV measurements. Further, six AlN substrates were irradiated with 8 MeV Al2+ at three fluences (1015, 1016, and 1017 ions/cm2) and two temperatures (300 °C and 500 °C). The $$d_{33}$$ for the six irradiated samples and one pristine sample were measured, and the measurement uncertainty was estimated based on five repeated tests. All samples were also measured by a commercial piezometer for comparison. The experimental results demonstrate that the piezoelectric coefficients obtained by LDV were about 0.8–1.16 pm/V lower than those obtained by the piezometer. With the compensation of the clamping effect, the corrected LDV values are similar to the piezometer results. Both show similar trends in all samples, which validates the feasibility of the proposed method for $$d_{33}$$ measurement. Based on the LDV results, the irradiated samples show a 12%–22% decrease in $$d_{33}$$ compared with the pristine samples. The samples irradiated under the same fluence at a higher temperature (500 °C) demonstrated a lower $$d_{33}$$ than those at 300 °C. The effect of the retro-reflective tape, sample temperature, and sample size on the $$d_{33}$$ measurement were also studied.« less
  5. Irradiation-induced Degradation of Surface Acoustic Wave Devices Fabricated on Bulk AlN

    Here, recent work to evaluate the prospects for surface acoustic wave (SAW) devices fabricated on bulk aluminum nitride (AlN) for elevated temperature and radiation environments is reported and discussed. The design and fabrication of an array of SAW devices using commercial wafers is described, including the non-standard fabrication approach taken to overcome the stress-induced warpage of the 50 mm diameter AlN substrates. Radio frequency performance characterization of the SAW devices, with resonance frequencies ranging from 0.5 GHz to 1.5 GHz, is described. The linear temperature coefficient of frequency (TCF) near room temperature was measured and is compared to theoretical resultsmore » from other investigators. Further, the effects of 8 MeV Al ion irradiation at 300°C and 500°C to damage levels of 0.01, 0.1 and 1 displacements per atom (dpa), as a proxy for neutron irradiation, was investigated. The ion irradiation damage was observed to decrease the SAW resonant frequency, and this effect is characterized and discussed. Significant degradation in the conductivity of the Ti/Al electrodes of the SAW devices was also observed and characterized. These experimental results provide a basis for further investigation of the prospects for development of SAW sensor devices in bulk AlN material for application in elevated temperature and radiation environments.« less
  6. Selective amorphization of SiGe in Si/SiGe nanostructures via high energy Si+ implant

    Here, the selective amorphization of SiGe in Si/SiGe nanostructures via a 1 MeV Si+ implant was investigated, resulting in single-crystal Si nanowires (NWs) and quantum dots (QDs) encapsulated in amorphous SiGe fins and pillars, respectively. The Si NWs and QDs are formed during high-temperature dry oxidation of single-crystal Si/SiGe heterostructure fins and pillars, during which Ge diffuses along the nanostructure sidewalls and encapsulates the Si layers. The fins and pillars were then subjected to a 3 × 1015 ions/cm2 1 MeV Si+ implant, resulting in the amorphization of SiGe, while leaving the encapsulated Si crystalline for larger, 65-nm wide NWsmore » and QDs. Interestingly, the 26-nm diameter Si QDs amorphize, while the 28-nm wide NWs remain crystalline during the same high energy ion implant. This result suggests that the Si/SiGe pillars have a lower threshold for Si-induced amorphization compared to their Si/SiGe fin counterparts. However, Monte Carlo simulations of ion implantation into the Si/SiGe nanostructures reveal similar predicted levels of displacements per cm3. Molecular dynamics simulations suggest that the total stress magnitude in Si QDs encapsulated in crystalline SiGe is higher than the total stress magnitude in Si NWs, which may lead to greater crystalline instability in the QDs during ion implant. The potential lower amorphization threshold of QDs compared to NWs is of special importance to applications that require robust QD devices in a variety of radiation environments.« less
  7. Understanding effects of chemical complexity on helium bubble formation in Ni-based concentrated solid solution alloys based on elemental segregation measurements

    Here, helium bubble formation and swelling were systematically studied in Ni-based concentrated solid solution alloys containing different numbers and types of elements. Our microscopy analysis showed that although increasing the alloy chemical complexity helps suppress bubble formation in general, there is no monotonic relationship between the bubble growth rate and the number of alloying elements. Certain elements (e.g., Fe and Pd) are more effective in suppressing bubble growth than others (e.g., Cr and Mn). Atom probe tomography was applied to accurately measure elemental segregation around bubbles, revealing unique effects of certain alloying elements on vacancy migration towards bubbles. More specifically,more » the high vacancy mobility via Cr sites leads to a large vacancy flux and an increased bubble size, while the high degree of atomic size mismatch introduced by Pd helps deflect vacancy flow away from bubbles and decrease the amount of swelling. The effects identified in this study provide new strategies to design concentrated solid solutions with superior resistance to swelling.« less
  8. Role of chemical disorder on radiation-induced defect production and damage evolution in NiFeCoCr

    Understanding chemical disorder in many concentrated solid solution alloys (CSAs) at the levels of electrons and atoms has attracted increasing attention as a path forward to reveal and identify underlying mechanisms for extraordinary mechanical properties and improved radiation tolerance. Single-phase NiFeCoCr CSA is a common base for many high-entropy alloys (HEAs) that have shown improved mechanical strength and radiation tolerance. In this study, defect production and damage evolution in NiFeCoCr under ion irradiation at room temperature to dose over 20 dpa are determined using ion channeling technique along both <100> and <110> directions utilizing multiple probing beam energies. The resultsmore » obtained from the multi-axial and multi-energy channeling analysis are compared with those previously obtained for Ni crystals irradiated under similar conditions. The influence of chemical complexity on defect production and clustering at early-stage under room temperature irradiation up to dose of 1 dpa is discussed based on positron annihilation spectroscopy results. Defect structure evaluation in Ni and NiFeCoCr is also discussed based on transmission electron microscopy results over a prolonged irradiation at both room and elevated temperatures. Compared with chemically complex NiFeCoCr, larger dislocation loops thus less lattice strain are expected to form in pure Ni. Moreover, the role of chemical disorder in this CSA is also investigated based on ab initio calculations using large supercells. Finally, to understand the impact of chemical complexity effect on defect structure evolution, this integrated research effort attempts to link the relatively large charge redistribution due to difference in valence electron counts resulting from alloying different 3d transition metal elements, moderate lattice distortion arising from similar adaptable atomic size, and notable suppressed or delayed damage evolution in NiFeCoCr.« less
  9. High Entropy Alloys: Irradiation

    High entropy alloys (HEAs) have been considered as structural materials for nuclear applications due to their promising mechanical properties and radiation resistance. For this purpose, irradiation-induced defect evolution and microstructure change have been characterized to evaluate the irradiation performance of different HEAs. This article reviews recent advances in understanding the irradiation response of HEAs, including the effect of disordered states on the defect energy landscape and defect evolution, irradiation-induced microstructure changes, void swelling, phase stability, mechanical properties under irradiation, as well as the He irradiation effects.
  10. Effect of thermochemical treatments on laser-induced luminescence spectra from strontium titanate: comparison with swift ion-beam irradiation experiments

    Results recently reported on the effect of thermochemical treatments on the (He-Cd) laser-excited emission spectra of strontium titanate (STO) are re-analyzed here and compared with results obtained under ion-beam irradiation. Contributing bands centered at 2.4 eV and 2.8 eV, which appear under laser excitation, present intensities dependent upon previous thermal treatments in oxidizing (O2) or reducing atmosphere (H2). As a key result, the emission band centered at 2.8 eV is clearly enhanced in samples exposed to a reducing atmosphere. From a comparison with the ionoluminescence data, it is concluded that the laser-excited experiments can be rationalized within a framework developedmore » from ion-beam excitation studies. In particular, the band at 2.8 eV, sometimes attributed to oxygen vacancies, behaves as expected for optical transitions from conduction-band (CB) states to the ground state level of the self-trapped exciton center. The band at 2.0 eV reported in ion-beam irradiated STO, and attributed to oxygen vacancies, is not observed in laser-excited crystals. As a consequence of our analysis, a consistent scheme of electronic energy levels and optical transitions can now be reliably offered for strontium titanate.« less
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