Peter Hosemann

Refractory high‐entropy alloys (RHEAs) are considered promising candidate materials for next‐generation nuclear reactors due to their superior mechanical strength, irradiation resistance, and thermal stability at high temperatures. However, the significant positive heat of mixing between refractory alloying elements and Cu, commonly used in cooling systems, poses challenges in forming composite structures. This study addresses the issue using a liquid metal dealloying (LMD) process. A precursor alloy (WTaVTi) with a directional dendrite‐interdendrite structure is fabricated and reacted with molten Cu at 1200 °C for 96 h. This approach produced a RHEA‐Cu composite with a stable interface between RHEA (W_31.5Ta_30.9V_21.4Ti_14.3) and Cu, featuring a spontaneously formed W‐rich interlayer that enhances interfacial bonding. The composite showed excellent irradiation resistance, with 30% less swelling under α‐ion irradiation than pure W. It also exhibited low thermal conductivity at room temperature, but reached ≈120 W m⁻¹·K⁻¹ at ≈650 °C, surpassing pure W. This temperature‐dependent rise in κ, with a positive gradient of +0.075 W m⁻¹·K⁻², is attributed to decreasing diffuse mismatch at elevated temperatures. The large‐scale reaction and stable microstructure achieved through LMD process highlight its industrial potential. This work offers a strategy for developing high‐performance materials by combining RHEA's radiation resistance with Cu's thermal conductivity for extreme environments.

Radiation-induced property changes in materials originate from the energy transfer from an incoming particle to the existing lattice, displacing atoms. The displaced atoms can cause the formation of extended defects including dislocation loops, voids, or precipitates. The non-equilibrium defects created during damage events determine the extent of these larger defects and are a function of dose rate, material, and temperature. However, these defects are transient and can only be probed indirectly. This work presents direct experimental measurements and evidence of irradiated non-equilibrium vacancy formation, where in situ positron annihilation spectroscopy was used to prove the generation of non-equilibrium defects in silicon.

The effect of thermal oxide layer on He implanted 316L stainless steel was studied to evaluate experimentally how thermal oxidation affects the diffusion and distribution of He in the material. In the case of thermal oxidation of a He implanted sample, with an increase in oxidation time, the max swelling height increases logarithmically as a function of time and finally saturates for all samples except for the lowest dose of implanted He. Concerning TEM results, two void regions are identified. Similar to the calculation, the total irradiated depth was around 250 nm and the large void region was formed around 100–150 nm depth. On the other hand, the small void region was observed immediately under oxide layer from the thermal oxidation. In contrast, there were no voids in the altered zone near the metal/oxide interface in the non-thermal oxidized/He implanted sample. This description of the phenomena was justified using the Kirkendall effect and the Point Defect Model.

Microstructural changes induced by helium implantation in materials lead to volumetric swelling and mechanical property changes. How these properties are linked and establishing direct relationships can be difficult due to the underlying material’s microstructure evolution. Some materials also experience a phase change due to irradiation damage making them even more complex to analyze. Here, single crystalline Si (100) was used to establish a relationship among these parameters. The swelling height as a function of implantation fluence can equally fit a linear relationship. Solely irradiation induced defects are observed at low fluence below 5.0 × 1016 ions/cm2. An abrupt amorphous and crystalline mixed layer of ∼200 nm thick within a highly damaged polycrystalline matrix is observed when implantation fluence exceeds 5.0 × 1016 ions/cm2, leading to the appearance of irradiation induced swelling and hardening behavior. As the fluence increases beyond 1.0 × 1017 ions/cm2, the amorphous layer expands in size and the bubble size distribution takes the form of a Gaussian distribution with a maximum size of up to 6.4 nm, which causes a further increase in the height of swelling. Furthermore, irradiation induced softening appeared due to the enlarged bubble size and amorphization.

Understanding the irradiation-induced defects in oxides is of interest for a wide range of applications. ZnO is an interesting oxide with mixed ionic and covalent bonding that contains a variety of point defect structures—making it an excellent model for studying irradiation-induced defects and their impact on properties. Here, we investigate the effects of neutron irradiation on the formation of defects and on the structural, optical, and electrical properties of ZnO single crystals. We observe the formation of vacancies and voids via positron annihilation spectroscopy. Neutron irradiation led to a significant deterioration of the ZnO structure and formed a high concentration of point defects, vacancy clusters, and voids with large disparities in their structure across variable irradiation times. It also led to significant changes in the optical properties and sample color. Irradiation for 444 h induced a high concentration of Cu acceptors as well as a high concentration of Ga donors. Temperature-dependent Hall effect measurements revealed the competing production of donors and acceptors and showed an increase in the slope of the carrier freeze-out curve with increasing irradiation dose. This work demonstrates the combined effects of neutron irradiation in producing a wide range of structural defects, impurities, and dopants in oxides and their enormous impact on modifying the oxide structure and both the optical and electronic properties. It particularly emphasizes the importance of considering the production of new impurities and dopants during the neutron irradiation of oxides.

Advancement of optoelectronic and high-power devices is tied to the development of wide band gap materials with excellent transport properties. However, bipolar doping (n-type and p-type doping) and realizing high carrier density while maintaining good mobility have been big challenges in wide band gap materials. Here P-type and n-type conductivity was introduced in β-Ga₂O₃, an ultra-wide band gap oxide, by controlling hydrogen incorporation in the lattice without further doping. Hydrogen induced a 9-order of magnitude increase of n-type conductivity with donor ionization energy of 20 meV and resistivity of 10⁻⁴ Ω.cm. The conductivity was switched to p-type with acceptor ionization energy of 42 meV by altering hydrogen incorporation in the lattice. Density functional theory calculations were used to examine hydrogen location in the Ga₂O₃ lattice and identified a new donor type as the source of this remarkable n-type conductivity. Positron annihilation spectroscopy measurements confirm this finding and the interpretation of the experimental results. This work illustrates a new approach that allows a tunable and reversible way of modifying the conductivity of semiconductors and it is expected to have profound implications on semiconductor field. At the same time, it demonstrates for the first time p-type and remarkable n-type conductivity in Ga₂O₃ which should usher in the development of Ga₂O₃ devices and advance optoelectronics and high-power devices.

Atom probe tomography (APT) is a powerful technique to characterize buried three-dimensional nanostructures in a variety of materials. Accurate characterization of those nanometer-scale clusters and precipitates is of great scientific significance to understand the structure–property relationships and the microstructural evolution. The current widely used cluster analysis method, a variant of the density-based spatial clustering of applications with noise algorithm, can only accurately extract clusters of the same atomic density, neglecting several experimental realities, such as density variations within and between clusters and the nonuniformity of the atomic density in the APT reconstruction itself (e.g., crystallographic poles and other field evaporation artifacts). This clustering method relies heavily on multiple input parameters, but ideal selection of those parameters is challenging and oftentimes ambiguous. In this study, we utilize a well-known cluster analysis algorithm, called ordering points to identify the clustering structures, and an automatic cluster extraction algorithm to analyze clusters of varying atomic density in APT data. This approach requires only one free parameter, and other inputs can be estimated or bounded based on physical parameters, such as the lattice parameter and solute concentration. The effectiveness of this method is demonstrated by application to several small-scale model datasets and a real APT dataset obtained from an oxide-dispersion strengthened ferritic alloy specimen.

Nanostructured ferritic alloys are considered as candidates for structural components in advanced nuclear reactors due to a high density of nano-oxides (NOs) and ultrafine grain sizes. However, bimodal grain size distribution results in inhomogeneous NO distribution, or vice versa. Here, we report that density of NOs in small grains (<0.5 µm) is high while there are almost no NOs inside the large grains (>2 µm) before and after irradiation. After 6 dpa neutron irradiation at 385–430 °C, α′ precipitation has been observed in these alloys; however, their size and number densities vary considerably in small and large grains. In this study, we have investigated the precipitation kinetics of α′ particles based on the sink density, using both transmission electron microscopy and kinetic Monte Carlo simulations. It has been found that in the presence of a low sink density, α′ particles form and grow faster due to the existence of a larger defect density in the matrix. On the other hand, while α′ particles form far away from the sink interface when the sink size is small, Cr starts to segregate at the sink interface with the increase in the sink size. Additionally, grain boundary characteristics are found to determine the radiation-induced segregation of Cr.

This study suggests a new approach to diffusion bonding (DB) 316L stainless steel: a low-pressure procedure that includes a nickel interlayer. In this approach, relatively lower pressure is applied to the sample before the DB process, in contrast to the usual approach in which higher pressure is applied during the DB process. This new procedure was tested on mock-up 316L stainless steel tube-to-tubesheet joints, which simulated similar joints in coiled-tube heat-exchanger applications. This study confirms that the new procedure meets the overall success criteria, namely, a pull-out force exceeding the force required for tube rupture. It also shows that the DB joint is improved by the use of a Ni interlayer; the joint strength increased by approximately 33% for a 0.25 μm Ni interlayer and by approximately 18% for a 5 μm Ni interlayer. The joint cross sections were qualitatively examined using optical microscopy (OM) and scanning electron microscopy (SEM); the observations suggest that only portions of the interface were diffusion bonded, as a result of the low-pressure procedure and the surface roughness (due to the sample fabrication). The portions that were diffusion bonded, though, were sound, as characterized by the fact that the steel grains grew through the interface line to create a continuous metallographic structure.

Polymer nanocomposites containing nanoparticle fillers often have enhanced strength, stiffness, and toughness that are highly dependent on nanoparticle spatial distribution, which can be challenging to control in the limit of high nanoparticle loading. Solid superlattices formed from close-packed, ligand-coated inorganic nanocrystals can have high stiffness and large elastic recovery, although nanocrystals interact solely through van der Waals forces. We use polymer-grafted nanocrystals to make superlattices with versatile structural architecture and dimensions to investigate the effects of structural defects, film thickness, and polymer length on mechanical behavior. We find that the elastic response of the superlattice is large even when the arrangement of nanocrystals within the superlattice is perturbed, and that polymer conformation plays a large role in determining mechanical properties.

In response to the DOE Sunshot Initiative to develop low-cost, high efficiency CSP systems, UCLA is leading a multi-university research effort to develop new high temperature heat transfer fluids capable of stable operation at 800°C and above. Due to their operating temperature range, desirable heat transfer properties and very low vapor pressure, liquid metals were chosen as the heat transfer fluid. An overview of the ongoing research effort is presented.

Development of new liquid metal coolants begins with identification of suitable candidate metals and their alloys. Initial selection of candidate metals was based on such parameters as melting temperature, cost, toxicity, stability/reactivity Combinatorial sputtering of the down selected candidate metals is used to fabricate large compositional spaces (∼ 800), which are then characterized using high-throughput techniques (e.g., X-ray diffraction). Massively parallel optical methods are used to determine melting temperatures. Thermochemical modeling is also performed concurrently to compliment the experimental efforts and identify candidate multicomponent alloy systems that best match the targeted properties. The modeling effort makes use of available thermodynamic databases, the computational thermodynamic CALPHAD framework and molecular-dynamics simulations of molten alloys. Refinement of available thermodynamics models are performed by comparison with available experimental data. Characterizing corrosion in structural materials such as steels, when using liquid metals, and strategies to mitigate them are an integral part of this study. The corrosion mitigation strategy we have adopted is based on the formation of stable oxide layers on the structural metal surface which prevents further corrosion. As such oxygen control is crucial in such liquid metal systems. Liquid metal enhanced creep and embrittlement in commonly used structural materials are also being investigated. Experiments with oxygen control are ongoing to evaluate what structural materials can be used with liquid metals. Characterization of the heat transfer during forced flow is another key component of the study. Both experiments and modeling efforts have been initiated. Key results from experiments and modeling performed over the last year are highlighted and discussed.

We employ intense and short pulses of energetic lithium (Li⁺) ions to investigate the relaxation dynamics of radiation induced defects in single crystal silicon samples. Ions both create damage and track damage evolution simultaneously at short time scales when we use the channeling effect as a diagnostic tool. Ion pulses, ∼20 to 600 ns long and with peak currents of up to ∼1 A are formed in an induction type linear accelerator, the Neutralized Drift Compression eXperiment at Lawrence Berkeley National Laboratory. By rotating silicon (<100>) membranes of different thicknesses and changing the incident ion energy, the fraction of channeled ions in the transmitted beam could be varied. In preliminary experiments we find that the Li ion intensity is not high enough to generate overlapping cascades (in time and space) that would be necessary to measure a change in the shape of the current waveform of the transmitted ion beam. We discuss the concept of pump-probe type experiments with short ion beam pulses to access defect dynamics in materials and outline a path to increasing damage rates with heavier ions and by the application of longitudinal and lateral pulse compression techniques.

In order to increase the thermal efficiency and produce process heat for hydrogen production, the operating temperature of the heat-transfer fluid in thermal solar plants needs to increase, but to increase the operating temperature, new heat-transport liquids need to be evaluated. Liquid metals have been proposed as heat-transport fluids because of the large temperature ranges over which they remain liquid. One of the most studied liquid metals for non-solar applications has been lead-bismuth eutectic alloy (LBE), for the nuclear industry. The main challenge with using LBE as a coolant is that the major constituents of structural steels have high solubility in LBE. In this work, the challenges of using LBE as a high temperature heat-transport fluid are discussed, as well as initial results of high-temperature static corrosion tests of structural steels to evaluate their potential use in a thermal solar power plant.

Extended abstract of a paper presented at Microscopy and Microanalysis 2012 in Phoenix, Arizona, USA, July 29 – August 2, 2012.