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At least 19 records

Site-specific plan-view (S)TEM sample preparation from thin films using a dual-beam FIB-SEM

To fully evaluate the atomic structure, and associated properties of materials using transmission electron microscopy, examination of samples from three non-collinear orientations is needed. This is particularly challenging for thin films and nanoscale devices built on substrates due to limitations with plan-view sample preparation. In this work, a new method for preparation of high-quality, site-specific, plan-view TEM samples from thin-films grown on substrates, is presented and discussed. Here, it is based on using a dual-beam focused ion beam scanning electron microscope (FIB-SEM) system. To demonstrate the method, the samples were prepared from thin films of perovskite oxide BaSnO 3 grown on a SrTiO 3 substrate and metal oxide IrO 2 on a TiO 2 substrate, ranging from 20–80 nm in thicknesses using molecular beam epitaxy. While the method is optimized for the thin films, it can be extended to other site-specific plan-view samples and devices build on wafers. Aberration-corrected STEM was used to evaluate the quality of the samples and their applicability for atomic-resolution imaging and analysis.

BaSnO3

Sample Preparation Laboratory (SPL) Best Practices: CGD as the Primary Acceptance Method

The traditional paradigm applied to the construction of nuclear safety related systems, structures, and components (SSCs), like SPL, involves an owner/licensee hiring an EPC firm with an NQA 1 program to manage the engineering, procurement, and construction of the desired SSC. This traditional approach would have posed significant barriers to the successful completion of the SPL. As a smaller capital project, in the $\$$100–$\$$200 million range, there was concern that employing one of the larger EPC companies would escalate costs and extend the projected schedule beyond what would be feasible for the Department of Energy (DOE). The traditional acceptance method employed for nuclear facilities with credited safety functions requires the use of an EPC firm applying American Society of Mechanical Engineers (ASME) NQA 1 nuclear quality assurance (NQA) to accept safety SSCs. In lieu of this approach, INL elected to apply its own NQA 1 program to hire an EPC firm operating a commercial quality program. This method used commercial grade dedication (CGD) as outlined in NQA 1 which had not been applied at this scale. Use of the commercial supply chain was identified as a key factor to the successful completion of SPL. Favorable conditions enabling the use of CGD included: • INL serving as both the designer and the design authority • Design created by an NQA 1 qualified source • A mature CGD program • Availability of a CGD subject matter expert (SME) • A strong construction management program. This white paper elaborates on the methodology employed in the construction of the SPL, the successes achieved, and best practices implemented.

42 - ENGINEERING

Electron Microscopy Transfer System to Protect Atmosphere‐Sensitive Materials for Scanning Electron Microscopy Characterization

Atmosphere- and/or moisture-sensitive materials can be challenging to characterize using electron microscopy techniques due to sample preparation workflows that generally require exposure to ambient conditions. Here, we describe a novel preparation method that uses aluminum foil in combination with a commercial cryo-EM transfer system to circumvent undesired exposure to the atmosphere. First, hygroscopic MgCl 2 was used as a model material, and prepared samples (both protected and unprotected) were placed in a controlled-humidity environment (> 80% relative humidity) for various exposure lengths (circa seconds to hours). Following this, the effectiveness of the sample preparation method was determined by comparing qualitative photos and quantitative X-ray diffraction patterns between the two sample subsets. The combined results of these experiments suggest that the outlined preparation method effectively protects MgCl 2 from atmospheric contamination compared to MgCl 2 samples that had no protective measures taken. Finally, the preparation method was utilized to protect a highly hygroscopic crystalline BaO thin film for characterization via scanning electron microscopy, thereby demonstrating a functional application of the outlined preparation technique and an additional use for the commercial cryo-EM transfer system beyond its intended application.

atmosphere-sensitive materials

A New Method for Polishing Laminated Dissimilar Metals

Here, this paper presents a novel method for preparing metallographic samples of laminated dissimilar metals, specifically a layered structure of zirconium (Zr), vanadium (V), and tungsten (W), which pose a challenge due to their differing crystal structures and hardness levels. The work was motivated by the need to develop a cladding for tungsten targets in spallation neutron sources, where a zirconium face is applied over an interlayer of either vanadium or titanium to prevent the formation of brittle intermetallic compounds such as ZrW 2 . Traditional polishing techniques prove inadequate because each constituent metal requires a different polishing approach based on its unique material properties. The methodology outlined includes a sequential process involving conductive epoxy mounting, successive grinding and polishing with specific abrasives, and a final chemical-mechanical polish using a colloidal silica-based solution. Optical microscopy confirmed that this multi-step process successfully produced scratch-free surfaces and minimized surface relief across the different metal interfaces. Although developed for refractory metals, this approach shows promise for other layered structures comprised of transition metals, offering a meticulous yet effective technique for high-quality metallographic sample preparation.

Newberry, Daniel [Oak Ridge National Laboratory (O

Geometric control of magnetic domain morphology in electrodeposited Ni rich NiPt mesoscopic wires

In this paper, we study the electrodeposited Ni—Pt magnetic wires, exploring the mechanisms by which changes in geometry and composition influence the local magnetic structure. The samples were prepared by electrodeposition, their elemental composition was analyzed by energy dispersive X-ray spectroscopy, and phase analysis was carried out by an X-ray diffraction measurement. Magnetic force microscopy measurements, and magnetic force microscopy measurements in magnetic field were carried out to study the domain morphology of the prepared samples. Magnetization characteristics were measured via vibrating sample magnetometry mode of a superconducting quantum interference device. Here, the results were analyzed and compared with micromagnetic simulations. It is shown that a strong perpendicular magnetic anisotropy is responsible for the characteristic checkerboard-like surface magnetization patterns, which can be tuned by geometrical constriction and Ni content. Understanding these relationships provides insights into the design of magnetic materials with tailored properties for advanced applications, like magnetic sensors.

Binary alloy

Automation of Laser Plasma Focused Ion Beam Microscopy for Next-Gen Energy Materials

Automation can revolutionize the use of ultrafast laser ablation and plasma-focused ion beam (PFIB) techniques for high-throughput, reproducible cross-sectioning and various sample preparation in materials characterization. As these methods become essential for analyzing complex energy materials and next-generation devices, efficient, standardized workflows are needed to minimize variability and enhance precision. This work highlights our advancements in developing automated processes for sample preparation that integrates machine learning, workflow optimization, and large-scale data acquisition to improve efficiency and scalability in applications such as electrolyzers, photovoltaic cells, and microelectronics. To streamline cross-sectioning and lamella fabrication, we have implemented fully automated workflows that standardize laser ablation and PFIB milling sequences. These workflows incorporate pre-programmed protocols for material removal, alignment, and thinning, reducing user intervention and ensuring consistency across different sample types. Machine learning algorithms further enhance automation by predicting optimal milling strategies and adapting parameters based on material properties and sectioning requirements. This approach significantly improves throughput while maintaining the structural integrity of prepared samples for high-resolution imaging and analysis, including transmission electron microscopy. Beyond sample preparation, our automation platform enables the acquisition of large, high-resolution datasets through serial sectioning, image alignment, and 3D reconstruction. These automated routines facilitate multi-scale characterization, capturing structural and compositional details from the nanoscale to the device level. By reducing variability and increasing efficiency, our automated approach enhances defect analysis, failure diagnostics, and process optimization, accelerating advancements in materials research and device engineering.

36 MATERIALS SCIENCE

Characterization of Tank 9H Annulus Sample in Support of Residual Material Inventory Determinations

The Savannah River National Laboratory (SRNL) was requested by Savannah River Mission Completion (SRMC) to provide sample preparation and characterization of the Tank 9H annulus sample in support of Residual Material Inventory Determinations. One Tank 9H sample in three vials [HTF-9-25-13, HTF-9-25-14 and HTF-9-25-15], with each vial containing approximately 200 mL of the Tank 9H annulus salt solution, were delivered to the SRNL Shielded Cells for sample preparation and characterizations in February 2025. The density of the “as-received” solution contained in each of the three Tank 9H annulus sample vials were determined followed by a solid-liquid separation on each one using 0.45-micron Nalgene® nylon filter membranes. The resulting filtrates were combined to form the Tank 9H annulus sample with a total volume of about 600 mL. The combined wet solid fractions, about a total of 4.8 grams of salt material, remaining on the filter membranes were air-dried in the Shielded Cells for 72 hours. The total weight of the air-dried solids was 2.1 grams. These air-dried solids were washed with deionized water (DI water) at a phase ratio of 60 mL DI water/gram of solids to recover insoluble solids, if any. No visible or measurable quantity of insoluble solids were recovered after DI water washing of the air-dried solids because the air-dried solids completely dissolved in the DI water. The solid fraction-wash water was not combined with the 600 mL of the filtrate solution, and the resulting solution was not screened or analyzed for radionuclides. Aliquot sample volumes of the undiluted Tank 9H annulus sample were sent to the SRNL analytical services groups for radionuclides, elementals, anions and total mercury analysis by various methods including radiochemical separations/counting methods, inductively coupled plasma-atomic emission spectroscopy (ICP-AES), and Inductively Coupled Plasma Mass Spectroscopy (ICP-MS) and special preparations. All sample analyses were performed in triplicate. This report presents the analytical characterization results for the Tank 9H annulus sample. The results are also reported where analytical methods yielded additional analytes, other than those requested by SRMC. In the characterization of the Tank 9H annulus sample, the detection limits for all the analytes, as specified in the Technical Task Request (TTR) and Task Technical and Quality Assurance Plan (TTQAP), were met.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W

Integrative Multi-PTM Proteomics Reveals Dynamic Global, Redox, Phosphorylation, and Acetylation Regulation in Cytokine-treated Pancreatic Beta Cells

Studying regulation of protein function at a systems level necessitates an understanding of the interplay among diverse post-translational modifications (PTMs). A variety of proteomics sample processing workflows are currently used to study specific PTMs but rarely characterize multiple types of PTMs from the same sample inputs. Method incompatibilities and laborious sample preparation steps complicate large-scale physiological investigations and can lead to variations in results. The single-pot, solid-phase-enhanced sample preparation (SP3) method for sample cleanup is compatible with different lysis buffers and amenable to automation, making it attractive for high-throughput multi-PTM profiling. Herein, we describe an integrative SP3 workflow for multiplexed quantification of protein abundance, cysteine thiol oxidation, phosphorylation, and acetylation. The broad applicability of this approach is demonstrated using cell and tissue samples, and its utility for studying interacting regulatory networks is highlighted in a time-course experiment of cytokine-treated ß-cells. We observed a swift response in global regulation of protein abundances consistent with rapid activation of JAK-STAT and NF-?B signaling pathways. Regulators of these pathways as well as proteins involved in their target processes displayed multi-PTM dynamics indicative of a complex cellular response stages: acute, adaptation, and chronic (prolonged stress). PARP14, a negative regulator of JAK-STAT, had multiple co-localized PTMs that may be involved in intraprotein regulatory crosstalk. Our workflow provides a high-throughput platform that can profile multi-PTMomes from the same sample set, which is valuable in unraveling the functional roles of PTMs and their co-regulation.

proteomics, PTM, automation, SP3, cysteine thiol o

Strategies for preparing and analyzing thin passive films with atom probe tomography

Atom probe tomography provides a unique, three-dimensional map of elemental and isotopic distributions over a wide range of materials with near-atomic scale resolution and is particularly strong at analyzing buried interfaces within materials. However, it is much more difficult to apply atom probe to the analysis of nanoscale surface films, such as those formed during alloy passivation, where unique challenges persist for sample preparation and data collection. Here, we present sample preparation strategies involving the deposition of a < 100 nm capping layer that enables reliable characterization of thin passive films approximately 2–5 nm thick formed on binary and multi-principal element alloys via atom probe tomography. Several capping layer materials (Pt, Ti, Ni/Cr bi-layer) and deposition methods are contrasted. Our results indicate a sputtered Ni/Cr bi-layer enables the characterization of the entire passive film and concentration profiles that can easily be interpreted to clearly distinguish base alloy/passive film/capping layer interfaces. Lastly, we highlight ongoing challenges and opportunities for this experimental approach.

Kautz, Elizabeth J. [University of Florida]

Machine learning enables reconstruction of past fire regimes from charcoal-derived fire intensity and fuel composition

Background Fire is a foundational ecological process that shapes ecosystem structure, diversity, and resilience. Quantifying paleofire regime attributes such as frequency, severity, and intensity is essential for understanding the historical range of variability in fire behavior and its ecological effects. While frequency and severity are often reconstructed in paleofire studies, quantitative reconstructions of fire intensity remain limited. Recent work has shown that maximum pyrolysis temperature—a proxy for fire intensity—and plant species type can be inferred from charcoal using transmission Fourier-transform infrared (FTIR) spectroscopy. However, the sample preparation for transmission FTIR is destructive and time-consuming, limiting application and reuse of materials for other analyses. We evaluated reflectance FTIR spectroscopy as a non-destructive alternative for reconstructing combustion temperature and plant species from laboratory-generated charcoal. We also examined the influence of contrasting airflow environments (ambient air versus nitrogen-rich) on pyrolysis temperature and plant species reconstruction prediction accuracies and compared predictive performance between a novel, neural network–based deep learning model with the traditional modern analogue technique (MAT) using k-nearest neighbor functions. As proof of concept, we apply our enhanced methodology to ancient charcoal to demonstrate applicability at improving long-term fire regime reconstructions and the ability to link paleofire records with contemporary fire ecology. Results Our analysis shows that transmission and reflectance FTIR spectra yield comparable spectral profiles. However, sample preparation for reflectance FTIR is minimal and non-destructive, unlike transmission FTIR which is destructive. We demonstrate that oxygen environments improved reconstruction accuracy relative to nitrogen-rich conditions. Finally, our deep learning neural network (DL) achieved testing accuracies of 98.7% for temperature and 96.2% for species identification, outperforming MAT’s k-NN approach (89.8% and 65.9%, respectively). A Shapley importance analysis identified 5 key spectral regions that greatly influenced the model’s temperature or species categorization. When applied to ancient charcoal, our results show historic fires from the most recent past primarily burned at low intensities (400–500 °C), reflective of natural fire regimes in ponderosa pine forests. Our results corroborate charcoal morphology data that suggests all ancient charcoal originated from burned woody plant types. Conclusions By combining reflectance FTIR spectroscopy with a deep learning approach, we provide the first accuracies high enough to confidently identify both species and temperature from laboratory-produced charcoal, improving quantitative reconstructions of fire intensity and fuel composition from paleofire records. This opens a wide range of research into the link between fire and larger drivers (i.e., climate or human) and greater ecological understanding of fire regimes beyond that of burn scars or recent observations. These methodological improvements have direct relevance for fire management by improving interpretation of historical fire behavior, informing fuel–fire relationships, and providing a scalable analytical framework applicable to both long-term ecological studies and contemporary fire science.

54 ENVIRONMENTAL SCIENCES

Destructive Analysis of TRISO Particles: Crush/Burn/Leach Followed by Davies-Gray Titration and IDMS

The accurate accounting of nuclear materials is a cornerstone of international nuclear safeguards. One emerging challenge in this domain is the fabrication of TRIstructural ISOtropic (TRISO) particle fuels. Although these innovative fuel forms are critical for advanced reactor applications, their robust refractory ceramics and coating compositions present significant obstacles to destructive analysis (DA) methods. Ensuring full and quantitative recovery from these particles is essential for accurate mass accountancy. The current study was initiated to address these challenges, first by validating a previously established destructive method developed by Oak Ridge National Laboratory (ORNL) for the quantitative recovery of uranium from TRISO particles and then following that process with uranium content determination through isotope dilution mass spectrometry (IDMS) and Davies-Gray titration. This study expands on the scope of a digestive method that was developed under the Advanced Gas Reactor Fuel Development and Qualification program and is currently implemented in both the Coated Particle Fuel Development Laboratory and Irradiated Fuels Examination Laboratory at ORNL. The success of the previous Advanced Gas Reactor work relied on developing a DA method to evaluate the fabrication process and reactor experiments. The methodology described in this report was designed to rigorously investigate the efficacy of the crush/burn/leach sample preparation of TRISO particles; it aims to quantify uranium recovery while also assessing the effects of TRISO constituents (e.g., silicon and zirconium) on analytical precision and accuracy. By comparing the results from the titration method and IDMS, we sought to determine whether existing analytical procedures accepted by the International Atomic Energy Agency (IAEA) could be effectively translated to TRISO fuel forms. The team employed an approach that involved processing replicate TRISO samples, optimizing the milling (i.e., crushing) step and performing serial leaches. The elemental composition of the analytical samples was examined to prepare for interference studies in the second year of this project. The integration of gamma spectrometry to verify residual uranium activity further strengthened the validation. Statistical methods were applied to the collected data to evaluate the uncertainties arising from sampling, sample preparation and uranium quantification. These uncertainties were then compared to the IAEA’s international target values (ITVs). Additional data collected in upcoming project work will strengthen the uncertainty estimates. Ultimately, it is hoped that this project will contribute materially to the body of work related to characterization of TRISO based fuels for the purpose of material accountancy and its applications to international safeguards.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Preparing for successful protein crystallization experiments

Crystal-based structural methods, including X-ray crystallography, are frequently utilized for the determination of high-resolution structures of biomolecules. All crystal-based diffraction methods first require the preparation of biomolecular crystals, and careful sample preparation for crystallization experiments can increase the frequency of success. In this article, strategies to optimize factors that can impact crystallization are presented, from which buffers and reducing agents are most favorable to which crystallization techniques could be used.

36 MATERIALS SCIENCE

Toward Automated Plasma Focus Ion Beam Instrument Calibration for Materials Processing [Poster]

To accelerate the transition to autonomous focused ion beam (FIB) microscopy, we require an objective figure of merit (FOM) for assessing calibration. For our purposes, these FOMs related to beam astigmatism, quad, and focus. Intelligent calibration integrated into scripted workflows will enable fully automated sample preparation workflows that produce higher quality samples with less operator time.

97 MATHEMATICS AND COMPUTING

Thermoreflectance Detection of Point Defects Resulting from Focused Ion Beam Milling

Focused ion beam (FIB) milling is a commonly used tool for nanoscale material processing, such as for transmission electron microscopy (TEM) sample preparation, or the creation of fiducial markers prior to other processes and measurements. During milling, a high energy ion beam is used to remove material via sputtering. The expelled target material may return to the sample surface however, affecting subsequent measurements. Beam spreading or irradiation due to neutral gallium may also irradiate a larger area than intended. Extensive research has explored the effects of FIB milling on the prepared TEM sample, but few have looked at the effects of milling on the properties of the sample surrounding the milled region. We use multiple pump-probe laser-based techniques (time domain thermoreflectance and steady-state thermoreflectance) to measure the spatial extent of FIB-induced surface/subsurface changes on a series of silicon wafers milled at multiple currents and doses. We supplement these measurements with high-resolution scanning transmission electron microscopy, energy dispersive X-ray spectroscopy, stylus profilometry, and time-of-flight secondary ion mass spectroscopy. We find a sample surface affected by the FIB up to 1 mm from where milling occurred, with a notable dependence on the ion beam current. We also note remarkably high sensitivity to surface defects using the thermoreflectance metrologies, including detection where other measurements failed.

defects

Characterization of Tank 15H Sample in Support of Preliminary Cease Waste Removal and Closure Mode Determination

The Savannah River National Laboratory (SRNL) was requested by Savannah River Mission Completion (SRMC) to provide sample preparation and analysis of Tank 15H characterization samples. These samples follow an interest in exploring avenues to condense the extensive sampling of the Tank Closure process. One such pathway would be to collect a sample during an earlier waste removal campaign for analysis to determine comparability to the later residual tank inventory determined through Residual Material sampling and characterization prior to grouting. Six Tank 15H samples (HTF-15-24-9, HTF- HTF-15-24-10, HTF-15-24-11, HTF-15-24-12, HTF&#x2;15-24-13, and HTF-15-24-14) were delivered to SRNL in May of 2024. These six Tank 15H samples were taken as close as possible to the solids layer of the Tank 15H. These six Tank 15H samples were combined to form one composite sample for characterization due to the lack of sufficient solids fraction.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W

Microstructural evaluation of thin-wall sections of 316L stainless steel produced by laser powder-bed fusion processing

The synthesis of thin wall sections that are only 0.4 mm thick is achieved with LPBF AM. Sample preparation is optimized using metallographic polishing to produce samples with only 0.3 um rms roughness for scanning electron microanalysis with EBSD and EDS. A fully austenitic 316L phase is found without evidence of secondary phases. Unlike some AM products that can readily evidence composition segregation due to solute rejection as attributable to temperature gradients within the solidification

Jankowski, Alan F. [Sandia National Laboratories (

Uncertainty improvement of 22 Na based radioactive tracer dilution for determining total mass of pyroprocessing molten salt systems by 154 Eu removal

To determine the total salt mass of the molten salt systems for pyroprocessing spent nuclear fuels, a 22 Na based radioactive tracer dilution was studied in Idaho National Laboratory in recent years. This 22 Na based RTD technique was deemed feasible, but due to the gamma energy peak of 22 Na coinciding with one of the energy peaks of 154 Eu radioisotope in the molten salt, the uncertainty of the 22 Na radioactivity in the 22 Na-spiked salt samples was quite high. To improve the uncertainty of the 22 Na based RTD technique, we proposed to chemically remove the 154 Eu of the salt samples by DGA resin for gamma spectroscopy. The effectiveness of removing 154 Eu on uncertainty improvement was evaluated. Furthermore, it was found that (1) the 154 Eu fission product effect on the uncertainty and detection limit can be effectively eliminated by chemically removing the 154 Eu during the salt sample preparation and (2) the uncertainty of 22 Na radioactivity in the salt samples for electrorefining was significantly improved from 13% to 2%, showing the potential of practical engineering application of 22 Na based RTD as a safeguards technique for molten salt systems for pyroprocessing spent nuclear fuels.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS