Michael Nastasi

The management of irradiation defects is one of key challenges for structural materials in current and future reactor systems. To develop radiation tolerant alloys for service in extreme irradiation environments, the Fe self-ion radiation response of nanocomposites composed of amorphous silicon oxycarbide (SiOC) and crystalline Fe(Cr) were examined at 10, 20, and 50 displacements per atom damage levels. Grain growth in width direction was observed to increase with increasing irradiation dose in both Fe(Cr) films and Fe(Cr) layers in the nanocomposite after irradiation at room temperature. However, compared to the Fe(Cr) film, the Fe(Cr) layers in the nanocomposite exhibited ~50% less grain growth at the same damage levels, suggesting that interfaces in the nanocomposite were defect sinks. Moreover, the addition of Cr to α-Fe was shown to suppress its grain growth under irradiation for both the composite and non-composite case, consistent with earlier molecular dynamic (MD) modeling studies.

The management of radiation defects and insoluble He atoms represent key challenges for structural materials in existing fission reactors and advanced reactor systems. To examine how crystalline/amorphous interface, together with the amorphous constituents affects radiation tolerance and He management, we studied helium bubble formation in helium ion implanted amorphous silicon oxycarbide (SiOC) and crystalline Fe composites by transmission electron microscopy (TEM). The SiOC/Fe composites were grown via magnetron sputtering with controlled length scale on a surface oxidized Si (100) substrate. These composites were subjected to 50 keV He+ implantation with ion doses chosen to produce a 5 at% peak He concentration. TEM characterization shows no sign of helium bubbles in SiOC layers nor an indication of secondary phase formation after irradiation. Compared to pure Fe films, helium bubble density in Fe layers of SiOC/Fe composite is less and it decreases as the amorphous/crystalline SiOC/Fe interface density increases. Our findings suggest that the crystalline/amorphous interface can help to mitigate helium defect generated during implantation, and therefore enhance the resistance to helium bubble formation.

Damage caused by implanted helium (He) is a major concern for material performance in future nuclear reactors. We use a combination of experiments and modeling to demonstrate that amorphous silicon oxycarbide (SiOC) is immune to He-induced damage. By contrast with other solids, where implanted He becomes immobilized in nanometer-scale precipitates, He in SiOC remains in solution and outgasses from the material via atomic-scale diffusion without damaging its free surfaces. Furthermore, the behavior of He in SiOC is not sensitive to the exact concentration of carbon and hydrogen in this material, indicating that the composition of SiOC may be tuned to optimize other properties without compromising resistance to implanted He.

The impact of neutron irradiation, in the energy range of ∼0.025 eV, on amorphous semiconducting partially dehydrogenated boron carbide (a-B10C2+xHy) on silicon p-n heterojunction diodes was investigated. The heterojunction devices were created by synthesizing a-B10C2+xHy via plasma enhanced chemical vapor deposition on n-type silicon. Unlike many electronic devices, the performance of the a-B10C2+xHy heterojunction diode improved with neutron irradiation, in spite of the large neutron cross section of 10B. There is also increased charge carrier lifetime of more than 200% with modest neutron irradiation of approximately 2.7 × 108 to 1.08 × 109 neutrons/cm2.

Temperature dependent He-irradiation-induced ion-beam mixing between amorphous silicon oxycarbide (SiOC) and crystalline Fe was examined with a transmission electron microscope (TEM) and via Rutherford backscattering spectrometry (RBS). The Fe marker layer (7.2 ± 0.8 nm) was placed in between two amorphous SiOC layers (200 nm). The amount of ion-beam mixing after 298, 473, 673, 873, and 1073 K irradiation was investigated. Both TEM and RBS results showed no ion-beam mixing between Fe and SiOC after 473 and 673 K irradiation and a very trivial amount of ion-beam mixing (~2 nm) after 298 K irradiation. At irradiation temperatures higher than 873 K, the Fe marker layer broke down and RBS could no longer be used to quantitatively examine the amount of ion mixing. The results indicate that the Fe/SiOC nanocomposite is thermally stable and tends to demix in the temperature range from 473 to 673 K. For application of this composite structure at temperatures of 873 K or higher, layer stability is a key consideration.

The plasma-enhanced chemical vapor (PECVD) co-deposition of pyridine and 1,2 dicarbadodecaborane, 1,2-B ₁₀ C ₂ H ₁₂ (orthocarborane) results in semiconducting boron carbide composite films with a significantly better charge extraction than plasma-enhanced chemical vapor deposited semiconducting boron carbide synthesized from orthocarborane alone. The PECVD pyridine/orthocarborane based semiconducting boron carbide composites, with pyridine/orthocarborane ratios ~3:1 or 9:1 exhibit indirect band gaps of 1.8 eV or 1.6 eV, respectively. These energies are less than the corresponding exciton energies of 2.0 eV–2.1 eV. The capacitance/voltage and current/voltage measurements indicate the hole carrier lifetimes for PECVD pyridine/orthocarborane based semiconducting boron carbide composites (3:1) films of ~350 µ s compared to values of ⩽35 µ s for the PECVD semiconducting boron carbide films fabricated without pyridine. The hole carrier lifetime values are significantly longer than the initial exciton decay times in the region of ~0.05 ns and 0.27 ns for PECVD semiconducting boron carbide films with and without pyridine, respectively, as suggested by the time-resolved photoluminescence. These data indicate enhanced electron–hole separation and charge carrier lifetimes in PECVD pyridine/orthocarborane based semiconducting boron carbide and are consistent with the results of zero bias neutron voltaic measurements indicating significantly enhanced charge collection efficiency.