Results for “structures annealing” — Page 39

DOE OSTI2022

Hydrogen Transport from Dielectrics to poly-Si/SiOx Passivating Contacts Measured by Mass Spectrometry and Vibrational Spectroscopy

We demonstrate the relationship between Si solar cell passivation and hydrogen content of various passivating films, including hydrogenated amorphous silicon (a-Si:H), aluminum oxide (Al2O3), silicon nitride (SiNx) and combinations thereof. Through isotopic studies using quadrupole mass spectrometry (QMS), Fourier transform infrared spectroscopy (FTIR), and Raman spectroscopy, we determine how hydrogen content and stability within each type of film relates to final passivation quality of solar cell test structures. Si solar cells using polycrystalline silicon on silicon oxide (poly-Si/SiOx) passivating contacts are at the forefront of Si solar cell research and emerging as top performers within industrial production. Performance of passivating contact Si solar cells is largely determined by a parameter known as the open-circuit voltage Voc, which directly relates to material quality within the bulk of the device and at surfaces. High Voc is achieved when defects within the bulk crystalline silicon (c-Si) and at interfaces are passivated, preventing them from acting as charge carrier recombination centers. One of the most important means of passivating defects within Si solar cells is via hydrogenation, injecting the cells with large amounts of H to satisfy dangling bonds in the bulk and at interfaces. Hydrogen is especially important in deactivating a prevalent defect in industrial p-type devices which leads to decreased device performance over long-term exposure to light, called light-induced degradation (LID). Some of the most common materials used to supply H to devices are a-Si:H, Al2O3, and SiNx, which can contain very large amounts of H. Upon annealing at elevated temperatures, the hydrogen becomes mobile enough to find and disable defect sites. However, too much hydrogen can also be problematic, sometimes leading to an effect called light and elevated temperature induced degradation (LeTID). It has been shown that these films passivate the interfaces of poly-Si passivating contacts differently, leading to differing performance. Though Al2O3 is a well-defined dielectric material, SiNx can have many different values of x depending on precursor gases and deposition conditions. We observe different FTIR and Raman spectra from different SiNx over a range of x values films to determine the bonding environments within them and further correlate the relative concentrations of Si, N, and H to the stability of H within SiNx and the passivation performance of each film. Because deuterium is chemically identical to hydrogen within these systems, but gives different signals in FTIR and Raman spectroscopy as well as in QMS, isotopic substitution can be used as an excellent tool to probe the H within films. In addition to measuring the H and D bonding within films using FTIR and Raman spectroscopy, we will use such isotopic experiments to observe H and D movement out of these hydrogenating films at elevated temperatures using QMS to determine the stability of H bonding within such systems. With these films characterized based on elemental composition, we will relate such measurements to passivation quality of these films and combinations thereof on poly-Si/SiOx contact structures using quasi-steady state photoconductance decay measurements to obtain implied open-circuit voltage (iVoc) and saturation current density J0 values. Such investigations into the performance of different passivating films and film stacks will lead to greater understanding of dielectrics in semiconductor devices, further improvements in passivated contact design, and eventually, greater proliferation of renewable solar energy worldwide.

Al2O3↗

DOE OSTI2023

The dependence of tungsten fuzz layer thickness and porosity on tungsten deposition rate and helium ion fluence

Abstract Fuzz formation on a heated tungsten surface in the presence of a helium-containing plasma and tungsten deposition source was investigated. Tungsten samples were exposed at 1123 K to pure helium plasma with ion incident energy of 76 eV, W/He ion flux ratio of ∼ 0.4 × 10 − 4 , and varied helium ion fluence from 0.18 to 3.4 × 10 26 m −2 . Fuzz thickness was measured by cross-sectional scanning electron microscopy to increase from 0.22 to 15 µ m with increasing helium ion fluence. No indication of saturation in fuzz thickness at high fluence was observed, in contrast to fuzz produced on a tungsten surface without tungsten deposition. Additional tungsten samples were exposed at 1123 K to pure helium plasma with ion incident energy of 76 eV, helium ion fluence of ∼ 3.4 × 10 26 m −2 , and varied W/He ion flux ratio from 0.26 to 3.0 × 10 − 4 . Fuzz thickness increased from 7.5 to 120 µ m with increasing W/He ion ratio. A final sample exposed at 1123 K to a mixed helium-deuterium plasma with ion incident energy of 76 eV, helium ion fluence of 0.18 × 10 26 m −2 , and W/He ion flux ratio of 2.2 × 10 − 4 developed nearly identical fuzz structures to that developed in a pure He plasma. As a function of deposited tungsten fluence, all results were found to trace out a single layer-growth curve given by a power law relation, indicating that fuzz thickness is independent of the W/He ion flux ratio in the range investigated and independent of any deuterium present in the plasma. As a result, for tungsten plasma facing walls in magnetic fusion devices at 1000–2000 K with 10 −4 W/He ion flux ratio, fuzz with thicknesses greater than hundreds of microns may form in as little as 10 4 s (in the absence of ELM-induced erosion or annealing), and may more significantly affect its thermophysical properties than fuzz generated without a tungsten deposition source.

Physics↗

DOE OSTI2020

Temperature-dependent growth of hexagonal and monoclinic gallium sulfide films by pulsed-laser deposition

We demonstrate the selective, pulsed-laser deposition of hexagonal GaS and monoclinic Ga2S3 films on sapphire substrates from a single Ga 2 S 3 target in high-vacuum conditions. Growth at substrate temperatures below 550 °C causes GaS film formation, which indicates non-stoichiometric transfer from the target to the film. Surprisingly, stoichiometric transfer occurs at substrate temperatures above 650 °C with monoclinic Ga 2 S 3 as the preferred, higher S-content phase. Through a series of growth and annealing experiments, we show that GaS nucleation under S-deficient conditions leads to the preferred growth of this layered, hexagonal phase below 550 °C. Furthermore, GaS films annealed above 650 °C under high vacuum are transformed to Ga 2 S 3 , reflecting the greater stability of the monoclinic phase. By first growing Ga 2 S 3 at a higher temperature and subsequently growing GaS at a lower temperature, we can fabricate GaS/Ga 2 S 3 heterostructures in a single growth process.

36 MATERIALS SCIENCE↗

DOE OSTI2021

β -Technetium: An allotrope with a nonstandard volume-pressure relationship

In this work, we report the synthesis and structure of the second allotrope of technetium, β-Tc. Transformative pathways are accessed at extreme conditions using the laser-heated diamond anvil cell and confirmed with in situ synchrotron x-ray diffraction and Raman spectroscopy. βTc is fully recoverable to ambient conditions, although counter to our DFT calculations predicting a face-centered-cubic lattice, we observe a tetragonal structure (I4/mmm) that exhibits further tetragonal distortion with pressure. β-Tc has an expanded volume relative to the hcp ground state phase, that when doped with nitrogen has an unexpected volume lowering. Such anomalous behavior is possibly indicative of a rare electronic phase transition in a 4d element.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Templated Growth and Passivation of Vertically Oriented Antimony Selenide Thin Films for High-Efficiency Solar Cells in Substrate Configuration

Antimony selenide (Sb 2 Se 3 ) is a promising low-cost photovoltaic material with a 1D crystal structure. The grain orientation and defect passivation play a critical role in determining the performance of polycrystalline Sb 2 Se 3 thin-film solar cells. In this work, a seed layer is introduced on a molybdenum (Mo) substrate to template the growth of a vertically oriented, columnar Sb 2 Se 3 absorber layer by closed space sublimation. By controlling the grain orientation and compactness of the Sb 2 Se 3 seeds, obtain high-quality Sb 2 Se 3 absorber layers with passive Sb 2 Se 3 /Mo interfaces is obtained, which in turn improve the transport of photoexcited charge carriers through the absorber layer and its interfaces. Post-deposition annealing of absorber layers in ambient air is further utilized to passivate the defects in Sb 2 Se 3 and enhance the quality of the front heterojunction. As a result of systematic processing optimization, Sb 2 Se 3 planar heterojunction solar cells are fabricated in substrate configuration with a champion power conversion efficiency of 8.5%.

14 SOLAR ENERGY↗

DOE OSTI2020

An Electron Backscatter Diffraction Analysis of Grain Boundary Initiated Discontinuous Precipitation in U-10Mo

The effect of varied thermomechanical processing on discontinuous precipitation (DP) in U-10Mo was investigated, with specific emphasis on understanding the role of grain boundary misorientation in DP. Varied prior homogenization heat treatment and thermomechanical processing resulted in differences in both the fraction of DP and the colony width, and was attributed to variations in the grain boundary misorientation distribution. Regardless of the degree of DP-based transformation, extensive growth of DP colonies was dominant on 30°–45° misorientation boundaries. Interestingly, misorientation histograms of the deformed and annealed specimens suggest the processing steps involved may have inhibited DP colony growth along a small fraction of these high angle boundaries. Large-area electron backscatter diffraction montages coupled with high resolution mapping suggest symmetric {110}-type interfaces may be important considerations for mitigating extensive DP growth in this alloy system.

Discontinuous Precipitation, Uranium, Electron Bac↗

DOE OSTI2020

Materials and technological processes for High-Gradient accelerating structures: new results from mechanical tests of an innovative braze-free cavity.

Pure oxygen-free high-conductivity copper is a widely used material for manufacturing accelerating cavities working at room temperature. Several studies attempted to explain limitations associated with the maximum allowed field gradients and the behaviour of vacuum RF breakdown in copper accelerating structures through generation and movement of dislocations under stresses associated with RF electric and magnetic fields. Pure copper and also copper alloys undergo mechanical and thermal treatments to be hardened and strengthened during manufacturing, although their mechanical properties significantly change after heating above 590°C. High temperature brazing and diffusion bonding are assembly methods widely used to manufacture ultra-high vacuum accelerating devices. However, these processes, occurring at about 800–1000°C, significantly affect the mechanical properties of copper and copper alloys. We introduce here a novel Tungsten Inert Gas welding procedure, which is fast and keeps the high-gradient surfaces of the cavity and other components well below the copper annealing temperature. This process may be successfully used to manufacture copper-based accelerating components. This technology further preserves the hardness and cleanliness of copper in order to achieve the maximum accelerating gradient.

47 OTHER INSTRUMENTATION↗

DOE OSTI2021

Formation of a Ti–Cu(111) single atom alloy: Structure and CO binding

A single atom Ti–Cu(111) surface alloy can be generated by depositing small amounts of Ti onto Cu(111) at slightly elevated surface temperatures (~500 to 600 K). Here, scanning tunneling microscopy shows that small Ti-rich islands covered by a Cu single layer form preferentially on ascending step edges of Cu(111) during Ti deposition below about 400 K but that a Ti–Cu(111) alloy replaces these small islands during deposition between 500 and 600 K, producing an alloy in the brims of the steps. Larger partially Cu-covered Ti-containing islands also form on the Cu(111) terraces at temperatures between 300 and 700 K. After surface exposure to CO at low temperatures, reflection absorption infrared spectroscopy (RAIRS) reveals distinct C–O stretch bands at 2102 and 2050 cm –1 attributed to CO adsorbed on Cu-covered Ti-containing domains vs sites in the Ti–Cu(111) surface alloy. Calculations using density functional theory (DFT) suggest that the lower frequency C–O stretch band originates specifically from CO adsorbed on isolated Ti atoms in the Ti–Cu(111) surface alloy and predicts a higher C–O stretch frequency for CO adsorbed on Cu above subsurface Ti ensembles. DFT further predicts that CO preferentially adsorbs in flat-lying configurations on contiguous Ti surface structures with more than one Ti atom and thus that CO adsorbed on such structures should not be observed with RAIRS. The ability to generate a single atom Ti–Cu(111) alloy will provide future opportunities to investigate the surface chemistry promoted by a representative early transition metal dopant on a Cu(111) host surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Resolving atomic transport through iron oxide under irradiation using isotopic tracers

Structural materials in nuclear environments are exposed to complex and harsh conditions, including high temperatures, corrosive solutions, and irradiation. Material stability and likewise degradation are fundamentally controlled by atomic transport mechanisms. Here, we investigate the influence of radiation-induced, non-equilibrium point defect populations on mass transport within model oxide systems using isotopic tracers and atom probe tomography. An isotopically labelled hematite (a-Fe2O3) film was synthesized with 16O- and 18O-rich layers (>30nm and 10 nm, respectively) sequentially deposited via molecular beam epitaxy. One region of the film was proton irradiated to ~0.1 dpa at 450°C, and regions outside the beam spot provided a non-irradiated control of thermal annealing only. 3D APT was used to directly visualize the elemental and O-isotopic redistribution following both thermal and combined thermal and irradiation conditions. Complementary scanning transmission electron microscopy (STEM) was also employed to study the microstructural evolution. Error function fits of the 18O-concentration profiles enabled quantification of diffusion coefficients.

isotopic tracers, diffusion, proton irradiation, h↗

DOE OSTI2021

Thermal stability and diffusion characteristics of ultrathin amorphous carbon films grown on crystalline and nitrogenated silicon substrates by filtered cathodic vacuum arc deposition

Amorphous carbon (a-C) films are widely used as protective overcoats in many technology sectors, principally due to their excellent thermophysical properties and chemical inertness. The growth and thermal stability of sub-5-nm-thick a-C films synthesized by filtered cathodic vacuum arc on pure (crystalline) and nitrogenated (amorphous) silicon substrate surfaces were investigated in this study. Samples of a-C/Si and a-C/SiN x /Si stacks were thermally annealed for various durations and subsequently characterized by high-resolution transmission electron microscopy (TEM) and electron energy loss spectroscopy (EELS). The TEM images confirmed the continuity and uniformity of the a-C films and the 5-nm-thick SiN x underlayer formed by silicon nitrogenation using radio-frequency sputtering. The EELS analysis of cross-sectional samples revealed the thermal stability of the a-C films and the efficacy of the SiNx underlayer to prevent carbon migration into the silicon substrate, even after prolonged heating. The obtained results provide insight into the important attributes of an underlayer in heated multilayered media for preventing elemental intermixing with the substrate, while preserving the structural stability of the a-C film at the stack surface. An important contribution of this investigation is the establishment of an experimental framework for accurately assessing the thermal stability and elemental diffusion in layered microstructures exposed to elevated temperatures.

42 ENGINEERING↗

DOE OSTI2022

Structure characterization and steam oxidation performance of U 3 Si 2 with Zr alloying additions

Research and development of high uranium density fuels supports the on-going effort to enhance reactor technology, safety, performance, and economics. Among high uranium density fuels, U 3 Si 2 is a favored fuel candidate due to its higher uranium density and improved thermal conductivity when compared to traditional UO 2 . While U 3 Si 2 demonstrates an improved fuel economy, it suffers from rapid degradation when exposed to water at T > 300°C. In order for U 3 Si 2 to be implemented in water cooled reactors, the water reaction must be understood and mitigated. Reported here is the performance of Zr alloying additions to U 3 Si 2 exposed to high temperature steam oxidation environments. Here, the investigation shows that homogenization heat treatment contributes to a delayed onset of oxidation and an improved homogeneity throughout the arc-melt fabricated alloyed compositions. Of the pre- and post-annealed samples, the post-annealed 7 vol% Zr addition exhibited the highest onset temperature of oxidation. A preliminary computational investigation to complement the experimental analysis assesses the solubility of Zr in U 3 Si 2 and its incorporation in the crystal lattice.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Nb3Sn Coating of Twin Axis Cavity and Other Complex SRF Cavity Structures

In the field of Accelerator Science, for the low cost and increased quality factor, thin films coated niobium cavities are used in the modern SRF research. Within the potential substances, Nb3Sn has shown higher critical temperature than niobium. Here the tin vapor diffusion method is used as the preferred technique to coat niobium cavities. So far, only elliptical cavities have been coated with Nb3Sn and this technique has not yet been applied to cavities with complex geometries, which are also helpful in the accelerator science field. The Half-wave resonator could provide us data across frequencies of interest for particle accelerators world wide. Similarly the Twin axis cavity proposed for Energy Recovary Linac (ERL) applications could benefit from Nb3Sn coating. But with their advanced geometries, increased area, more number of ports and hard to reach areas, a different coating approach is needed to provide a uniform coating of Nb3Sn. We used twin axis cavity to optimize the coating technique and followed a low temperature annealing to further improvement of the thin film quality by low temperature annealing as a post coating method. With these we could expand the current coating system at JLab to coat complex cavity models

Tiskumara, Jayendrika↗

DOE OSTI2025

Chemical Interaction of Palladium in Uranium Oxycarbide Nuclear Fuel Kernel

Chemical Interaction of Palladium in Uranium Oxycarbide Nuclear Fuel Kernel Jana Howard1,3, Guang Yang3, Haiyan Zhao1*, Patrick Warren4, Tiankai Yao3, Steven Cavazos4 Elizabeth Sooby Wood4*, Ching-heng Shiau2 1 University of Idaho, Environmental Science, Idaho Falls, Idaho, USA 2 Boise State University, Microscopy and Characterization Suite, Idaho Falls, Idaho, USA 3 Idaho National Laboratory, Idaho Falls, Idaho, USA 4 University of Texas San Antonio, Department of Physics and Astronomy, San Antonio, Texas, USA *Corresponding author: haiyanz@uidaho.edu; elizabeth.soobywood@utsa.edu Tri-structural Isotropic (TRISO) particle fuel is the preferred choice for the newest and next-generation high-temperature nuclear reactors due to its robust construction [1]. The fuel design effectively contains fission products inside the particle at extremely high temperatures [2]. However, the effect of transition metal fission products on fuel performance and structural integrity remains largely unknown, creating uncertainties in predicting fuel performance and potential failure mechanisms [2]. For example, palladium (Pd) has a strong tendency to form intermetallic phases with uranium (U). These new phases tend to be hard and brittle which could lead to fracture of fuel kernel during irradiation [3,4]. Pd is not normally produced in high concentrations in normal fission reactions however, driving the production of Pd into the locality of a Uranium Oxycarbide (UCO) nuclear fuel provides an opportunity to closely observe the diffusion and chemical interactions. This study focuses on detailed transmission electron microscopy characterization of the intermetallic phases formed by the interaction between a UCO kernel and a Pd bar after annealing at 1100 °C for 100 hours. Figure 1 provides an overview of the UCO kernel in contact with the Pd bar. The UCO-Pd sample surface was examined using a Focused Ion Beam (FIB) Quanta 3D FEG FEI in VCD detector mode at 10kV, 83pA to reveal surface features. Several key surface features in the interaction region were observed including: (1) a small area with dendritic microstructure, (2) color contrast near the UCO kernel and Pd boundary, and (3) darker and lighter regions throughout the sample surface. To analyze diffusion behavior, FIB was used to prepare lamellae from five different areas of the UCO-Pd sample, as well as one for the as-received sample. These lamellae were examined using a Scanning Transmission Electron Microscope ThermoFisher Spectra 300 (STEM-Spectra). Energy Dispersive Spectroscopy results confirmed the diffusion between the UCO fuel and Pd bar. Figure 2 shows the identified phases of UC, UO2, and Pd dispersed throughout the interaction region. It was also found that the Pd concentration decreases as the radial distance from the UCO-Pd interface increases. The Pd concentration was 36.93% atomic fraction 11µm from the interaction region then decreased to 7.51% atomic fraction at 257 µm away from the interaction region. Figure 3 shows how concentrations of U and Pd vary across the interaction zone, highlighting the extent of diffusion. This study confirms that Pd interacts with surrounding material to form U-Pd phase and diffusion zones. These diffusion zones vary in composition depending on its radial distance from the point of contact with the Pd bar. These findings contribute to a deeper understanding of the fission product behavior in high temperature nuclear fuels, aiding in the prediction and mitigation of potential fuel degradation mechanisms. A B C Fig. 1. SEM micrographs of UCO fuel kernel in contact with solid Pd bar and the lift out locations. Figure 1A shows UCO fuel kernel in contact with solid Pd bar. Figure 1B shows a higher magnification image of the UCO fuel-Pd interaction zone. Figure 1C shows lift out sites for the lamellae. A B C Fig 2. EDS maps reveal the distribution of U, O, and Pd in location 3. Figure 2A shows the distribution of uranium. Figure 2B shows the distribution of oxygen. Figure 2C shows the distribution of palladium. A B C Fig 3. Palladium and uranium concentration across interaction zone in location 2. Figure 3A shows EDS map of lift out number 2. Figure 3B shows a zoomed in EDS map taken from the interaction zone. Figure 3C shows a line graph of uranium and palladium concentrations across the interaction zone. References: 1. B.E. Wells, N.R. Phillips, K.J. Geelhood. Pacific West Laboratory. (2021). TRISO Fuel: Properties and Failure Modes. https://www.nrc.gov/docs/ML2117/ML21175A152.pdf (Accessed January 16, 2025). 2. American Nuclear Society. TRISO Fuel Development Progresses in INL, ORNL. https://www.gen-4.org/gif/upload/docs/application/pdf/2014-03/nov13nn_fuel_reprint.pdf (Accessed January 16, 2025) 3. Clark R.A., M.A. Con

36 - MATERIALS SCIENCE↗

DOE OSTI2025

Chemical Interaction of Palladium in Uranium Oxycarbide Nuclear Fuel Kernel

Chemical Interaction of Palladium in Uranium Oxycarbide Nuclear Fuel Kernel Jana Howard1,3, Guang Yang3, Haiyan Zhao1*, Patrick Warren4, Tiankai Yao3, Steven Cavazos4 Elizabeth Sooby Wood4*, Ching-heng Shiau2 1 University of Idaho, Environmental Science, Idaho Falls, Idaho, USA 2 Boise State University, Microscopy and Characterization Suite, Idaho Falls, Idaho, USA 3 Idaho National Laboratory, Idaho Falls, Idaho, USA 4 University of Texas San Antonio, Department of Physics and Astronomy, San Antonio, Texas, USA *Corresponding author: haiyanz@uidaho.edu; elizabeth.soobywood@utsa.edu Tri-structural Isotropic (TRISO) particle fuel is the preferred choice for the newest and next-generation high-temperature nuclear reactors due to its robust construction [1]. The fuel design effectively contains fission products inside the particle at extremely high temperatures [2]. However, the effect of transition metal fission products on fuel performance and structural integrity remains largely unknown, creating uncertainties in predicting fuel performance and potential failure mechanisms [2]. For example, palladium (Pd) has a strong tendency to form intermetallic phases with uranium (U). These new phases tend to be hard and brittle which could lead to fracture of fuel kernel during irradiation [3,4]. Pd is not normally produced in high concentrations in normal fission reactions however, driving the production of Pd into the locality of a Uranium Oxycarbide (UCO) nuclear fuel provides an opportunity to closely observe the diffusion and chemical interactions. This study focuses on detailed transmission electron microscopy characterization of the intermetallic phases formed by the interaction between a UCO kernel and a Pd bar after annealing at 1100 °C for 100 hours. Figure 1 provides an overview of the UCO kernel in contact with the Pd bar. The UCO-Pd sample surface was examined using a Focused Ion Beam (FIB) Quanta 3D FEG FEI in VCD detector mode at 10kV, 83pA to reveal surface features. Several key surface features in the interaction region were observed including: (1) a small area with dendritic microstructure, (2) color contrast near the UCO kernel and Pd boundary, and (3) darker and lighter regions throughout the sample surface. To analyze diffusion behavior, FIB was used to prepare lamellae from five different areas of the UCO-Pd sample, as well as one for the as-received sample. These lamellae were examined using a Scanning Transmission Electron Microscope ThermoFisher Spectra 300 (STEM-Spectra). Energy Dispersive Spectroscopy results confirmed the diffusion between the UCO fuel and Pd bar. Figure 2 shows the identified phases of UC, UO2, and Pd dispersed throughout the interaction region. It was also found that the Pd concentration decreases as the radial distance from the UCO-Pd interface increases. The Pd concentration was 36.93% atomic fraction 11µm from the interaction region then decreased to 7.51% atomic fraction at 257 µm away from the interaction region. Figure 3 shows how concentrations of U and Pd vary across the interaction zone, highlighting the extent of diffusion. This study confirms that Pd interacts with surrounding material to form U-Pd phase and diffusion zones. These diffusion zones vary in composition depending on its radial distance from the point of contact with the Pd bar. These findings contribute to a deeper understanding of the fission product behavior in high temperature nuclear fuels, aiding in the prediction and mitigation of potential fuel degradation mechanisms. A B C Fig. 1. SEM micrographs of UCO fuel kernel in contact with solid Pd bar and the lift out locations. Figure 1A shows UCO fuel kernel in contact with solid Pd bar. Figure 1B shows a higher magnification image of the UCO fuel-Pd interaction zone. Figure 1C shows lift out sites for the lamellae. A B C Fig 2. EDS maps reveal the distribution of U, O, and Pd in location 3. Figure 2A shows the distribution of uranium. Figure 2B shows the distribution of oxygen. Figure 2C shows the distribution of palladium. A B C Fig 3. Palladium and uranium concentration across interaction zone in location 2. Figure 3A shows EDS map of lift out number 2. Figure 3B shows a zoomed in EDS map taken from the interaction zone. Figure 3C shows a line graph of uranium and palladium concentrations across the interaction zone. References: 1. B.E. Wells, N.R. Phillips, K.J. Geelhood. Pacific West Laboratory. (2021). TRISO Fuel: Properties and Failure Modes. https://www.nrc.gov/docs/ML2117/ML21175A152.pdf (Accessed January 16, 2025). 2. American Nuclear Society. TRISO Fuel Development Progresses in INL, ORNL. https://www.gen-4.org/gif/upload/docs/application/pdf/2014-03/nov13nn_fuel_reprint.pdf (Accessed January 16, 2025) 3. Clark R.A., M.A. Con

36 - MATERIALS SCIENCE↗

DOE OSTI2024

Report Summarizing the Mechanical Properties of a Large ODS Ferritic Alloy Ingot by Forging at High Temperatures for Future Mother Tube Production

Oxide dispersion strengthened (ODS) ferritic alloys are considered the benchmark fuel cladding and core structural material in advanced nuclear energy reactors that require high-temperature strength and creep properties and resistance to radiation damage. The ODS ferritic alloys including 14YWT are produced by mechanical alloying (MA), which is time-consuming and is associated with high manufacturing costs that are not beneficial to being used in advanced nuclear energy reactors. This report summarizes the accomplishments in FY24 in the INM program for producing an ODS ferritic alloy by high-deformation, high-temperature processing of reactive and ferritic alloy powders for advanced reactor fuel cladding applications. Following four hot forging experiments, it was concluded that several significant challenges were encountered that were difficult to overcome. These challenges were related to using high annealing temperatures for pressure assisted sintering processes to produce dense microstructures, but the high annealing temperatures result in long range diffusion of Ti through the bcc Fe lattice and react with the YIG particles that are distributed on the prior surfaces of the ferritic alloy powders. In addition, it was determined that the high deformations induced by forging at high temperatures were not very effective for fracturing the reactive YIG particles into smaller particles and distributing them into the interior of the ferritic alloy powders. Spark plasma sintering was attempted for shortening the time at high temperatures, which led to full densification but the microstructure characterization results still showed that Ti atoms diffused over long distances in the bcc Fe lattice and reacted with the YIG particles. Finally, a short 30 minute high intensity ball milling experiment was conducted on blended 14WT and YIG powders for inducing severe deformations that caused the initially spherical powders of 14WT decorated with the YIG particles on the surfaces to transform to flakes and fracturing of YIG particles into smaller particles that were incorporated into the bcc Fe lattice. Two forgings were performed with the high intensity milled powders: first annealing for 20 minutes at 850ºC followed by forging and second annealing for 20 minutes at 1,100ºC followed by forging. At 850ºC, Ti atoms are effectively immobile, thus allowing for densification albeit incomplete. The deformation by forging after annealing for 20 minutes at 1,100ºC favored dynamic recrystallization processes that led to nano-size grains with very high stored energy due to high dislocation density. The corresponding VH data showed significant hardening that correlated with estimated strengthening of ~1650 MPa. This hybrid processing approach combining high intensity ball milling of powder with annealing and forging showed the most promise for producing an oxide dispersing strengthened ferritic alloy.

36 MATERIALS SCIENCE↗

DOE OSTI2023

In situ spin coater for multimodal grazing incidence x-ray scattering studies

We present herein a custom-made, in situ, multimodal spin coater system with an integrated heating stage that can be programmed with spinning and heating recipes and that is coupled with synchrotron-based, grazing-incidence wide- and small-angle x-ray scattering. The spin coating system features an adaptable experimental chamber, with the ability to house multiple ancillary probes such as photoluminescence and visible optical cameras, to allow for true multimodal characterization and correlated data analysis. This system enables monitoring of structural evolutions such as perovskite crystallization and polymer self-assembly across a broad length scale (2 Å–150 nm) with millisecond temporal resolution throughout a complete thin film fabrication process. The use of this spin coating system allows scientists to gain a deeper understanding of temporal processes of a material system, to develop ideal conditions for thin film manufacturing.

47 OTHER INSTRUMENTATION↗

DOE OSTI2021

Reduction of the molecular hamiltonian matrix using quantum community detection

Abstract Quantum chemistry is interested in calculating ground and excited states of molecular systems by solving the electronic Schrödinger equation. The exact numerical solution of this equation, frequently represented as an eigenvalue problem, remains unfeasible for most molecules and requires approximate methods. In this paper we introduce the use of Quantum Community Detection performed using the D-Wave quantum annealer to reduce the molecular Hamiltonian matrix in Slater determinant basis without chemical knowledge. Given a molecule represented by a matrix of Slater determinants, the connectivity between Slater determinants (as off-diagonal elements) is viewed as a graph adjacency matrix for determining multiple communities based on modularity maximization. A gauge metric based on perturbation theory is used to determine the lowest energy cluster. This cluster or sub-matrix of Slater determinants is used to calculate approximate ground state and excited state energies within chemical accuracy. The details of this method are described along with demonstrating its performance across multiple molecules of interest and bond dissociation cases. These examples provide proof-of-principle results for approximate solution of the electronic structure problem using quantum computing. This approach is general and shows potential to reduce the computational complexity of post-Hartree–Fock methods as future advances in quantum hardware become available.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Developing Efficient Perovskite/Silicon Tandem Devices

This project aims at developing highly efficient perovskite/silicon tandem solar cells by developing efficient perovskite top cells, silicon bottom cells, and monolithically integrating the subcells for highly efficient tandem solar cells. The project focused on increasing the efficiency of perovskite solar cells to 20% and understanding related materials science and device physics, as well as developing a compatible bottom high-efficiency c-Si solar cell. The perovskite cells with a wide bandgap of 1.61 eV and 1.84 eV are fabricated by a low-cost, low-temperature, scalable solution process on lower bandgap silicon bottom cells. The bandgaps of perovskite top cells have been tuned between 1.61 eV and 1.84 eV by composition engineering mainly through controlling the halide mixing ratio in perovskite materials. The efficiencies of the wide bandgap perovskite solar cells have been improved to an excellent efficiency of 21.0% for perovskites with a bandgap of 1.63 eV with increased grain size, reduced energy disorder at cathode contact, and defect passivation. We invented a solvent annealing approach with solvent vapor during thermal annealing to enlarge grain size of perovskite film which reduces the charge trap density and improves the device efficiency. Moreover, we discovered that the non-wetting surface could further increase the grain size for perovskite films, because non-wetting surface could prevent the formation of too dense nuclei from heterogeneous nucleation process. We proposed to reduce the energy disorder of organic charge extraction layer to reduce the power loss in perovskite cells. We pioneered defect passivation concept and techniques to suppress the charge non-radiative recombination in perovskite solar cells to boost the efficiency. For the silicon bottom cell development, different from the conventional silicon cell work under full illumination, the light available for the silicon bottom cell in tandem structure is mainly NIR region. We developed a NIR enhanced silicon cell with efficiency of 21.2% by applying a double-layer antireflection coating at the front side and a MgF2 back reflector layer at the rear side. For the perovskite/silicon tandem device, we achieved a highest reported power conversion efficiency of 25.4% in 2018, and further increased the efficiency up to 26.0% in 2019. The research on tandem solar cells focused on reducing reflection loss to <5% at spectrum of 300-1100 nm by antireflection layer, tuning the bandgap of perovskite film for matched current density between sub-cells, and utilizing a ITO layer between perovskite top cell and silicon bottom cell as interconnect layer without Voc loss. Finally, we developed a blading technique to fabricate perovskite films which produces perovskite solar cells with comparable or even superior efficiency to those made by non-scalable spin coating method. This paves the way for scaling up perovskite/silicon tandem solar cells using solution approach.

14 SOLAR ENERGY↗