Quantifying the atomic neighbourhoods in complex concentrated alloys
Here is presented that atom probe tomography unlocks the potential to precisely analyse the short-range ordering in a CoCrNi medium-entropy alloy.
36 MATERIALS SCIENCE↗
SEARCH · Engineering Papers
Results for “Atom probe tomography”
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Exploring the effects of molecular beam epitaxy growth characteristics on the temperature performance of state-of-the-art terahertz quantum cascade lasers
This study conducts a comparative analysis, using non-equilibrium Green’s functions (NEGF), of two state-of-the-art two-well (TW) Terahertz Quantum Cascade Lasers (THz QCLs) supporting clean 3-level systems. The devices have nearly identical parameters and the NEGF calculations with an abrupt-interface roughness height of 0.12 nm predict a maximum operating temperature (T max ) of ~ 250 K for both devices. However, experimentally, one device reaches a T max of ~ 250 K and the other a T max of only ~ 134 K. Both devices were fabricated and measured under identical conditions in the same laboratory, with high quality processes as verified by reference devices. The main difference between the two devices is that they were grown in different MBE reactors. Our NEGF-based analysis considered all parameters related to MBE growth, including the maximum estimated variation in aluminum content, growth rate, doping density, background doping, and abrupt-interface roughness height. From our NEGF calculations it is evident that the sole parameter to which a drastic drop in T max could be attributed is the abrupt-interface roughness height. We can also learn from the simulations that both devices exhibit high-quality interfaces, with one having an abrupt-interface roughness height of approximately an atomic layer and the other approximately a monolayer. However, these small differences in interface sharpness are the cause of the large performance discrepancy. This underscores the sensitivity of device performance to interface roughness and emphasizes its strategic role in achieving higher operating temperatures for THz QCLs. We suggest Atom Probe Tomography (APT) as a path to analyze and measure the (graded)-interfaces roughness (IFR) parameters for THz QCLs, and subsequently as a design tool for higher performance THz QCLs, as was done for mid-IR QCLs. Our study not only addresses challenges faced by other groups in reproducing the record T max of ~ 250 K and ~ 261 K but also proposes a systematic pathway for further improving the temperature performance of THz QCLs beyond the state-of-the-art.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Role of crystallographic orientation in atom probe analysis of Li-ion battery cathode materials
Using air-stable lithium cobalt oxide (LCO) as a prototypical system, we elucidate the role of crystallographic orientation and anisotropic transport in atom probe tomography (APT) for lithium transition metal oxide (LTMO) cathode materials.
Lin, Jr-Wen [Department of Materials Science and E↗
Improving luminescence response in ZnGeN 2 /GaN superlattices: defect reduction through composition control
Abstract Color-mixed (cm) light-emitting diodes (LEDs) are theoretically the most efficient white light emitters, projected to improve white light luminous efficacy by 34% compared to incumbent phosphor converted LEDs. Since white light technology is pervasive and essential, small improvements in LED technology can result in energy savings. However, cm-LEDs are not yet realized due to poor efficacy in green and amber emitting materials, a spectral region colloquially referred to as the Green Gap. ZnGeN 2 is nearly isostructural and closely lattice-matched to GaN and can be heteroepitaxially integrated with existing GaN devices; ZnGeN 2 /GaN hybrid structures are theorized to emit green (~530 nn) light with a spontaneous emission rate 4.6–4.9 times higher than traditional InGaN LEDs when incorporated into III-N LED structures. In this report we demonstrate the molecular beam epitaxy (MBE) growth of GaN and ZnGeN 2 superlattices, an important step towards realizing multiple quantum well structures required for efficient LEDs. Elemental analysis, including atom probe tomography, shows that Ga and Ge are observed in both ZnGeN 2 and GaN layers, degrading the structural uniformity. The lack of elemental abruptness also leads to increased defect luminescence and reabsorption of band edge luminescence. The source of unintentional Ga distributed throughout the ZnGeN 2 layers was identified as excess flux escaping from around the closed MBE shutter. The source of unintentional Ge, which tended to incorporate as a single delta-doped layer in GaN, was identified as Ge riding along the cyclical metal-rich Ga adlayer used for high quality GaN, incorporating during subsequent nitrogen-rich growth step. Modifying the growth strategy results in improved structural quality, elemental abruptness, and luminescence response. This realization of structurally and elementally abrupt interfaces demonstrates the potential of heteroepitaxially integrated binary and ternary nitrides for energy-relevant devices.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Roadmap on data-centric materials science
Science is and always has been based on data, but the terms ‘data-centric’ and the ‘4th paradigm’ of materials research indicate a radical change in how information is retrieved, handled and research is performed. It signifies a transformative shift towards managing vast data collections, digital repositories, and innovative data analytics methods. The integration of artificial intelligence and its subset machine learning, has become pivotal in addressing all these challenges. This Roadmap on Data-Centric Materials Science explores fundamental concepts and methodologies, illustrating diverse applications in electronic-structure theory, soft matter theory, microstructure research, and experimental techniques like photoemission, atom probe tomography, and electron microscopy. While the roadmap delves into specific areas within the broad interdisciplinary field of materials science, the provided examples elucidate key concepts applicable to a wider range of topics. The discussed instances offer insights into addressing the multifaceted challenges encountered in contemporary materials research.
36 MATERIALS SCIENCE↗
Shielded magnetic small-angle neutron scattering for characterization of radioactive samples
The development of a Pb-shielded fixture for the execution of a small-angle neutron scattering (SANS)-based workflow for interrogation of highly irradiated nuclear materials has been explored. The Pb shielding was specially designed to reduce the detected radioactivity from the specimen during SANS experiments, and the overall configuration is termed shielded magnetic SANS (SM-SANS). Two FeCrAl-based alloys, C35M and 125YF, were examined with the SM-SANS technique using a free-form size distribution locally monodisperse model in both the as-received and irradiated states. Quantitative values derived from the free-form size distribution were compared with atom probe tomography experiments. Microstructural and compositional parameters determined using the two characterization techniques were complements of each other. The results demonstrate that the SM-SANS technique is an effective means of characterizing nanoscale clustering in irradiated material systems and provides new avenues for investigating radioactive material microstructures.
FeCrAl↗
Hiperclust
This software leverages transfer learning to analyze atom probe tomography (APT) data. It is trained on synthetic data and then applies this knowledge to predict the optimal number of clusters for a given APT dataset. Initially, the software used preliminary clustering to estimate the general structure of the data. Based on this, it provides suggestions for key parameters like minimum cluster size and minimum number of points. These parameters are critical for algorithms like HDBSCAN, ensuring accurate cluster formation without the need for trial-and-error testing. The software runs on High-Performance computing (HPC) systems, enabling fast, scalable analysis of large APT datasets, ultimately saving time and improving the reliability of clustering outcomes.
Tang, Yalei [Idaho National Laboratory (INL), Idah↗
Machine Learning for Predictive Performance Analysis in Charged Particle Beam Tools
Imaging methods driven by probes, electrons, and ions have played a dominant role in modern science and engineering. Opportunities for machine vision and AI that focus on consumer problems like driving and feature recognition, are now presenting themselves for automating aspects of the scientific processes. This proposal aims to enable and drive discovery in ultra-low energy implantation by taking advantage of faster processing, flexible control and detection methods, and architecture-agnostic workflows that will result in higher efficiency and shorter scientific development cycles. Custom microscope control, collection and analysis hardware will provide a framework for conducting novel in situ experiments revealing unprecedented insight into surface dynamics at the nanoscale. Ion implantation is a key capability for the semiconductor industry. As devices shrink, novel materials enter the manufacturing line, and quantum technologies transition to being more mainstream. Traditional implantation methods fall short in terms of energy, ion species, and positional precision. Here we demonstrate 1 keV focused ion beam Au implantation into Si and validate the results via atom probe tomography. We show the Au implant depth at 1 keV is 0.8 nm and that identical results for low energy ion implants can be achieved by either lowering the column voltage, or decelerating ions using bias – while maintaining a sub-micron beam focus. We compare our experimental results to static calculations using SRIM and dynamic calculations using binary collision approximation codes TRIDYN and IMSIL. A large discrepancy between the static and dynamic simulation is found that is due to lattice enrichment with high stopping power Au and surface sputtering. Additionally, we demonstrate how model details are particularly important to the simulation of these low-energy heavy-ion implantations. Finally, we discuss how our results pave a way to much lower implantation energies, while maintaining high spatial resolution.
47 OTHER INSTRUMENTATION↗
Production of Creep-Resistant FeCrAl-ODS
Four ODS FeCrAl alloys with base alloy composition Fe-16Cr-4Al-2Mo-0.2Y (wt.%) were mechanically alloyed with minor additions of CeO 2 and Y 2 O 3 additions and were successfully extruded into rectangular-shaped bars. Two oxide compositions were explored, which were designated NC with oxide addition of 0.5CeO 2 plus 0.2Yin solution of the base alloy powder and PC with additions of 0.5CeO 2 and 0.7Y 2 O 3 to elevate the O level. The microstructure of both alloys revealed by SEM and EBSD to consist of very small grains with sizes of ~450-520 nm and weak texture components. Sub-size tensile specimens fabricated from both alloys were tensile tested from room temperature to 800ºC. The results for both alloys from room temperature to 400ºC showed very high strengths, but low ductilities, especially uniform strain. From 500ºC to 800ºC, the strengths decreased rapidly, and the ductilities increased significantly. The reason for the rapid decreases in tensile strengths above 500ºC for both alloys is not clear, but will require advanced characterization techniques including atom probe tomography, to determine the size and number density of the nano-size oxide particles, and TEM/EFTEM, for investigating the dispersion of nano-size oxide particles on grain boundaries to assess the Zener grain boundary pinning effect, which will hinder grain coarsening at high temperatures that may enhance the Hall Petch strengthening mechanism.
36 MATERIALS SCIENCE↗
Charpy Impact Characterization of Surveillance Specimens Harvested from Palisades High Fluence A-60 Capsule
Located on the shores of Lake Michigan, the Palisades Nuclear Generating Station (PNGS) was a nuclear power plant that operated in Covert Township, Michigan. The plant had a single pressurized water reactor that produced electricity for the region. The PNGS was shut down in 2022 after more than four decades of service. The PNGS included in its surveillance program a surveillance capsule, designated A-60, containing specimens of a weld metal with nickel content of about 1.36 wt% and copper content of about 0.25 wt%. The capsule was removed from its surveillance position in early 1995 and has been resident in the spent fuel pool since that time. This capsule was irradiated to a fluence of 1.96×10 20 n/cm 2 (E>1MeV) that is equivalent for more than 150 effective full power years (EFPYs) for the US reactor pressure vessel (RPV) fleet. The material is also of special interest because of its very high nickel content and potential for development of NiMnSi (nickel-manganese-silicon) precipitates. Combination of very high fluence and very high Ni and Cu content makes the material in this capsule of great interest as benchmark for currently developing embrittlement trend curves (ETC) aiming to predict embrittlement at high fluences. Multi-year efforts by the Light Water Reactor Sustainability (LWRS) Program personnel from the Materials Research Pathway (MRP) to harvest this capsule finally succeeded in 2023. As a result, the Westinghouse Electric Company (WEC) through contract with Oak Ridge National Laboratory (ORNL) came to PNGS site, retrieved the A-60 capsule, brought it to WEC Churchill hot cell facility, opened the capsule and sent all surveillance specimens in the capsule to ORNL for future characterization by July 2023. Total of 9 tensile and 48 Charpy specimens were inventoried in the ORNL hot cells. Testing plan has been developed based on available specimens. It includes hardness, tensile, Charpy impact, Mini-CT fracture toughness testing, in-situ thermal annealing, and microstructural characterization, including Atom Probe Tomography (APT). Charpy impact testing has been completed and results are presented in this report. Moreover, negotiations with Pressurized Water Reactors Owners Group (PWROG) and Westinghouse resulted in Westinghouse donating to ORNL a piece of archive weld and base metal such that unirradiated characterization of these materials can be performed as part of this project. Comparison of measured hardening and embrittlement has been performed and data are compared to available large database.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Development of PNNL’s Plutonium Metallography Capability
The goal of this project was to develop plutonium metallography capabilities and establish workflows for characterization at PNNL’s Radiological Processing Facility (RPL). Developing and expanding on this capability opens more opportunities for PNNL to better support science through collaborations with other labs, plants, and sites withing the Department of Energy Complex and through programs within the National Nuclear Security Administration. This project established metallography equipment in an air glovebox, polishing protocols, as well as radiological and facility controls and procedures so that gram quantities of plutonium metal could be analyzed on multiple characterization tools. Data was collected and analyzed on two different delta phase plutonium - Gallium samples and a calciothermically reduced alpha plutonium metal using a combination of optical and electron microscopy, powder X-ray diffraction, and atom probe tomography. This report highlights the metallography capabilities, some preliminary data collections, and plans at PNNL to support plutonium material science.
36 MATERIALS SCIENCE↗
Impact of Annealing on Superconducting Properties of Tantalum Thin Films
The pursuit for higher-coherence superconducting qubits has led to the adoption of new materials and innovative fabrication techniques. Among the commonly used superconducting materials, tantalum-based or tantalum-capped superconducting qubits have demonstrated the longest lifetimes, outperforming niobium devices even in the presence of their native oxides. Given the losses introduced by the surface oxide, one method to further improve performance is to reduce or eliminate the native oxide on tantalum through UHV annealing. In this work, we examine the effect of dissolved oxygen as a function of annealing temperature on the superconducting properties of tantalum thin films. Dissolved oxygen is quantified using atom probe tomography (APT) and secondary ion mass spectrometry (TOF-SIMS) and correlated with electromagnetic transport measurements performed using a Physical Property Measurement System (PPMS). This study observes that annealing decomposes the native oxide and drives oxygen diffusion into the film matrix. Increasing oxygen content decreases the superconducting transition temperature (Tc) and the residual resistivity ratio (RRR). The critical field decreases with the incorporation of oxygen, while the film’s coherence length decreases relatively by 5%. These results, as well as findings from ongoing studies linking fabrication processes to the structural and chemical properties of the superconducting film and Josephson junction, provide insight into effective strategies for improving the performance of superconducting devices.
Shinde, Maithilee [IIT, Chicago; Fermilab]↗
Thermodynamics and kinetics of core-shell versus appendage co-precipitation morphologies
What determines precipitate morphologies in co-precipitating alloy systems? We focus on alloys of two precipitating phases, with the fast-precipitating phase acting as heterogeneous nucleation sites for a second phase manifesting slower kinetics. Kinetic lattice Monte Carlo simulations show that the interplay between interfacial and ordering energies, plus active diffusion paths, strongly affect the selection of core-shell verses appendage morphologies. We study a FeCuMnNiSi alloy using the combination of atom probe tomography and simulations, and show that the ordering energy reduction of the MnNiSi phase heterogeneously nucleated on a pre-existing copper-rich precipitate exceeds the energy penalty of a predominantly Fe/Cu interface, leading to initial appendage, rather than core-shell, formation. Diffusion of Mn, Ni and Si around and through the Cu core towards the ordered phase results in subsequent appendage growth. We further show that in cases with higher primary precipitate interface energies and/or suppressed ordering, the coreshell morphology is favored.
Shu, Shipeng↗
Effects of Rhenium Addition on the Temporal Evolution of the Nanostructure and Chemistry of a Model Ni-Cr-Al Superalloy: Analysis of the Coarsening Behavior - 2
The temporal evolution of the nanostructure and chemistry of a model Ni-8.5 at.% Cr-10 at.% Al alloy with the addition of 2 at.% Re was studied using transmission electron microscopy and atom-probe tomography in order to measure the number density and mean radius of the y' (LIZ) precipitates and the chemistry of the y'-precipitates and the y (fcc)-matrix. In this article, the coarsening behavior of the y'-precipitates is discussed in detail and compared with the Umantsev-Olson model for multi-component alloys. In addition, the experimental results are evaluated with PrecipiCalc(TradeMark) simulations. The results show that the diffusivities of the solute elements play a major role in the coarsening behavior of the y'-precipitates and that the addition of Re retards the coarsening kinetics and stabilizes the spheroidal morphology of the precipitates by reducing the interfacial energy.
Yoon, Kevin E.↗
Compositional Pathways and Capillary Effects during Early-stage Isothermal Precipitation in a Nondilute Ni-Al-Cr Alloy
For a Ni-5.2 Al-14.2 Cr at.% alloy with moderate solute supersaturations, the compositional pathways, as measured with atom-probe tomography, during early to later stage y'(LI2)-precipitation (R = 0.45-10 nm), aged at 873 K, are discussed in light of a multi-component coarsening model. Employing nondilute thermodynamics, detailed model analyses during quasistationary coarsening of the experimental data establish that the y/y' interfacial free-energy is 22- 23+/-7 mJ/sq m. Additionally, solute diffusivities are significantly slower than model estimates. Strong quantitative evidence indicates that an observed y'-supersaturation of Al results from the Gibbs-Thomson effect, providing the first experimental verification of this phenomenon. The Gibbs-Thomson relationship, for a ternary system, as well as differences in measured phase equilibria with CALPHAD assessments, are considered in great detail.
Sudbrack, Chantal K.↗
Effects of Rhenium Addition on the Temporal Evolution of the Nanostructure and Chemistry of a Model Ni-Cr-Al Superalloy: Experimental Observations - 1
The temporal evolution of the nanostructure and chemistry of a model Ni-8.5 at.% Cr-10 at. % Al alloy, with the addition of 2 at.% Re, aged at 1073 K from 0.25 to 264 h, was studied. Transmission electron microscopy and atom-probe tomography were used to measure the number density and mean radius of the gamma prime (L1(sub 2) structure)-precipitates and the chemistry of the gamma prime-precipitates and the gamma (face-centered cubic)-matrix, including the partitioning behavior of all alloying elements between the gamma- and gamma prime-phases and the segregation behavior at gamma/gamma prime interfaces. The precipitates remained spheroidal for an aging time of up to 264 h and, unlike commercial nickel-based superalloys containing Re, there was not confined (nonmonotonic) Re segregation at the gamma/gamma prime interfaces.
Yoon, Kevin E.↗
Temporal Evolution of the Nanostructure and Phase Compositions in a Model Ni-Al-Cr Alloy
In a Ni-5.2 Al-14.2 Cr at.% alloy with moderate solute supersaturations and a very small gamma/gamma prime lattice parameter misfit, the nanostructural and compositional pathways during gamma prime(L12) precipitation at 873 K are investigated using atom-probe tomography, conventional transmission electron microscopy, and hardness measurements. Nucleation of high number densities (N(sub v) greater than 10(sup 23) per cubic meters) of solute-rich precipitates (mean radius = [R] = 0.75 nm), with a critical nucleus composition of Ni-18.3 plus or minus 0.9 Al-9.3 plus or minus 0.7 Cr at.%, initiates between 0.0833 and 0.167 h. With increasing aging time (a) the solute concentrations decay in spheroidal precipitates ([R] less than 10 nm); (b) the observed early-stage coalescence peaks at maximum N(sub v) in coincidence with the smallest interprecipitate spacing; and (c) the reaction enters a quasi-stationary regime where growth and coarsening operate concomitantly. During this quasi-stationary regime, the c (face-centered cubic)-matrix solute supersaturations decay with a power-law dependence of about -1/3, while the dependencies of [R] and N(sub v) are 0.29 plus or minus 0.05 and -0.64 plus or minus 0.06 at a coarsening rate slower than model predications. Coarsening models allow both equilibrium phase compositions to be determined from the compositional measurements. The observed early-stage coalescence is discussed in further detail.
Sudbrack, Chantal K.↗
Effects of Solute Concentrations on Kinetic Pathways in Ni-Al-Cr Alloys
The kinetic pathways resulting from the formation of coherent gamma'-precipitates from the gamma-matrix are studied for two Ni-Al-Cr alloys with similar gamma'-precipitate volume fractions at 873 K. The details of the phase decompositions of Ni-7.5Al-8.5Cr at.% and Ni-5.2Al-14.2Cr at.% for aging times from 1/6 to 1024 h are investigated by atom-probe tomography, and are found to differ significantly from a mean-field description of coarsening. The morphologies of the gamma'-precipitates of the alloys are similar, though the degrees of gamma'-precipitate coagulation and coalescence differ. Quantification within the framework of classical nucleation theory reveals that differences in the chemical driving forces for phase decomposition result in differences in the nucleation behavior of the two alloys. The temporal evolution of the gamma'-precipitate average radii and the gamma-matrix supersaturations follow the predictions of classical coarsening models. The compositional trajectories of the gamma-matrix phases of the alloys are found to follow approximately the equilibrium tie-lines, while the trajectories of the gamma'-precipitates do not, resulting in significant differences in the partitioning ratios of the solute elements.
Booth-Morrison, Christopher↗