High-energy Diffraction Microscopy Research Articles

Nanometer-thick molecular beam epitaxy Al films capped with in situ deposited Al2O3—High-crystallinity, morphology, and superconductivity

Achieving high material perfection in aluminum (Al) films and their associated Al/AlOx heterostructures is essential for enhancing the coherence time in superconducting quantum circuits. We grew Al films with thicknesses ranging from 3 to 30 nanometers (nm) epitaxially on sapphire substrates using molecular beam epitaxy (MBE). An integral aspect of our work involved electron-beam (e-beam) evaporation to directly deposit aluminum oxide (Al2O3) films on the freshly grown ultrathin epitaxial Al films in an ultra-high-vacuum (UHV) environment. This in situ oxide deposition is critical for preventing the oxidation of parts of the Al films, avoiding the formation of undesired native oxides, and thereby preserving the nm-thick Al films in their pristine conditions. The thicknesses of our Al films in the study were accurately determined; for example, coherence lengths of 3.0 and 20.2 nm were measured in the nominal 3.0 and 20 nm thick Al films, respectively. These Al films were epitaxially grown on sapphire substrates, showing an orientational relationship, denoted as Al(111)⟨21¯1¯⟩∥sapphire(0001)[21¯1¯0]. The Al/sapphire interface was atomically ordered without any interfacial layers, as confirmed by in situ reflection high-energy electron diffraction (RHEED) and cross-sectional scanning transmission electron microscopy (STEM). All sample surfaces exhibited smoothness with a roughness in the range of 0.1–0.2 nm. The Al films are superconducting with critical temperatures ranging from 1.23 to around 2 K, depending on the film thickness.

3D Reconstruction of a High-Energy Diffraction Microscopy Sample Using Multi-modal Serial Sectioning with High-Precision EBSD and Surface Profilometry

High-energy diffraction microscopy (HEDM) combined with in situ mechanical testing is a powerful nondestructive technique for tracking the evolving microstructure within polycrystalline materials during deformation. This technique relies on a sophisticated analysis of X-ray diffraction patterns to produce a three-dimensional reconstruction of grains and other microstructural features within the interrogated volume. However, it is known that HEDM can fail to identify certain microstructural features, particularly smaller grains or twinned regions. Characterization of the identical sample volume using high-resolution surface-specific techniques, particularly electron backscatter diffraction (EBSD), can not only provide additional microstructure information about the interrogated volume but also highlight opportunities for improvement of the HEDM reconstruction algorithms. In this study, a sample fabricated from undeformed “low solvus, high refractory” nickel-based superalloy was scanned using HEDM. The volume interrogated by HEDM was then carefully characterized using a combination of surface-specific techniques, including epi-illumination optical microscopy, zero-tilt secondary and backscattered electron imaging, scanning white light interferometry, and high-precision EBSD. Custom data fusion protocols were developed to integrate and align the microstructure maps captured by these surface-specific techniques and HEDM. The raw and processed data from HEDM and serial sectioning have been made available via the Materials Data Facility (MDF) at https://doi.org/10.18126/4y0p-v604 for further investigation.

Sulphuric precipitates in novel titanium-based, sulphur-bearing bulk metallic glass – a BMG composite?

ABSTRACT New titanium-based metallic glasses containing sulphur as a key element have recently been developed and are the subject of ongoing research related to the effects of sulphur introduction into glass-forming alloy systems. Here we report on the formation of sulphuric precipitates during solidification of a Ti40Zr35Cu17S8 alloy and on the occurrence of secondary intermetallic compound crystallization starting in sulphur-depleted zones around the precipitates. The alloy is a promising metallic glass for use as a structural and biomedical material as it shows a high yield strength and good corrosion resistance paired with a low density. The role of sulphur for the glass formation in the Ti-Zr-Cu-S system is discussed and specimens quenched into different structural states are investigated by means of high-energy synchrotron diffraction and electron microscopy. The electron microscopic findings reveal that sulphuric precipitates precede the crystallization of an intermetallic (Ti, Zr)2Cu phase, which is the primary phase when sulphur is not present in the system and thus lead to a higher glass-forming ability. The sulphuric precipitates are found in specimens of various casting thickness and differ in their volume percentages depending on the size of the cast sample, while the secondary phase (Ti, Zr)2Cu crystallizes heterogeneously in the interfaces between the sulphuric precipitates and the local matrix.

In situ measurement of three-dimensional intergranular stress localizations and grain yielding under elastoplastic axial-torsional loading

The three-dimensional grain-averaged response of solid bar samples under non-proportional (NP) elastoplastic axial-torsional loading was investigated using in situ high energy diffraction microscopy (HEDM) and companion crystal plasticity finite element (CPFE) modeling. Important stress metrics including applied shear (σθZ) and axial (σZZ) stress tensor components, stress and stress deviator tensor invariants (I1, J2, and J3), von Mises equivalent stress (σVMgrain), maximum resolved shear stress (mRSS), stress triaxiality (η), and lode angle parameter (θ‾) values were tracked for ∼ 300 grains under two different loading conditions: (1) Torsion-dominated loading (low NP) and (2) Tension-torsion loading (high NP) in equiatomic NiCoCr, a representative multicomponent face-centered cubic (FCC) superalloy. Overall, significant stress localizations existed within both samples as evidenced by the radial dependence of grain-resolved σθZ, σVMgrain , and J2; by comparison, I1, J3, η, and θ‾ metrics did not show discernible trends within the volume. These stress localizations reveal a complex interplay between axial and shear stress components (e.g., stress coupling) resulting in grain yielding near the sample surface largely driven by shear stress, whereas internal grain yielding was largely accommodated by axial stress. Grain-resolved stress localization trends were described well by the CPFE model, although some discrepancies in magnitude occurred, particularly for volumetric stress metrics (I1 and η) due to initial type II residual stress distributions. The superposition of initial residual stress states onto CPFE grain-resolved data significantly improved model accuracy for η. This suggests that residual stresses more strongly influence the simulation of volumetric rather than deviatoric (yield) stress metrics.

3D in-situ characterization of dislocation density in nickel-titanium shape memory alloys using high-energy diffraction microscopy

3D in-situ characterization of dislocation density in nickel-titanium shape memory alloys using high-energy diffraction microscopy

Four-dimensional microstructurally small fatigue crack growth in cyclically loaded nickel superalloy specimen

We nondestructively image a low-solvus high refractory (LSHR) nickel base specimen microstructure during cyclic loading to characterize crack propagation during the microstructurally small crack (MSC) growth regime. Micro-computed tomography (μCT) is used to characterize the material density and identify crack interfaces, while high-energy diffraction microscopy (HEDM) provides snapshots of the microstructural orientation field changes. From these measurements, data are computationally reconstructed and coregistered to describe the specimen’s configuration before load, before crack nucleation, and throughout the crack propagation/loading process. An MSC forms at a FIB-cut notch, which was previously placed to concentrate stress at the center of the specimen gauge, and propagates along a facet parallel to the local {111} crystallographic plane. Analysis of available crystallographic slip directions and measured point-to-point disorientation axes indicate probable single and coplanar slip activity along FCC octahedral planes within this region. Similar analyses of other crack propagation facets reveal generally slower growth along directions favoring zig-zag cross and codirectional cross slip, which are often disfavored at room temperature.

Deep learning for improving grain mapping from near-field high-energy diffraction microscopy

Deep learning for improving grain mapping from near-field high-energy diffraction microscopy

Crystallinity degradation and defect development in (AlxGa1−x)2O3 thin films with increased Al composition

We systematically analyzed the Al composition dependences of the structural properties of (AlxGa1−x)2O3 thin films grown on β-Ga2O3 (010) substrates. The crystal structure was characterized by x-ray diffraction, and the surface morphology was observed by reflection high-energy electron diffraction and atomic force microscopy. In the 100-nm-thick thin films, the crystallinity began to degrade and defects appeared on the surface when the Al composition x exceeded about 0.16. The defects developed mainly along the [201] direction and slightly along the [001] direction as x increased. The boundary where the thin film quality changed was close to a critical thickness curve calculated using the Matthews–Blakeslee model assuming the slip system of ⟨201⟩{102¯}.

Energy dissipation by grain boundary replacement during grain growth

The changes in both the grain boundary area and grain boundary energy that occur during grain growth have been measured in polycrystalline Ni using high energy diffraction microscopy. In addition to the reduction of grain boundary area, the average grain boundary energy decreases as higher energy grain boundaries are replaced by lower energy grain boundaries. This energy dissipation mechanism influences grain boundary migration and might explain the absence of a correlation between grain boundary curvature and migration velocity.Classical studies of isotropic grain growth in polycrystals have been based on the idea that grain boundary (GB) migration is driven by the product of the GB energy and curvature. [1,2] While support for this foundational concept is certainly found in studies of bicrystals [3] and simulations [4], recent experimental evidence contradicts this idea. When measured curvatures and velocities were compared in Ni [5] and SrTiO3, [6] they were found to be uncorrelated. Similar observations were reported for α-Fe, [7] where the measured constant of proportionality between curvature and velocity did not behave in expected ways. The purpose of this letter is to present evidence that, during grain growth, the replacement of higher energy GBs by lower energy boundaries dissipates energy by a mechanism that is not related to curvature. This reduction of the average GB energy represents an additional driving force for grain growth.For a GB network comprised of N triangular mesh elements of area ai, the total free energy (F) is:

Grain Boundary Migration in Polycrystals

Grain boundaries in polycrystalline materials migrate to reduce the total excess energy. It has recently been found that the factors governing migration rates of boundaries in bicrystals are insufficient to explain boundary migration in polycrystals. We first review our current understanding of the atomistic mechanisms of grain boundary migration based on simulations and high-resolution transmission electron microscopy observations. We then review our current understanding at the continuum scale based on simulations and observations using high-energy diffraction microscopy. We conclude that detailed comparisons of experimental observations with atomistic simulations of migration in polycrystals (rather than bicrystals) are required to better understand the mechanisms of grain boundary migration, that the driving force for grain boundary migration in polycrystals must include factors other than curvature, and that current simulations of grain growth are insufficient for reproducing experimental observations, possibly because of an inadequate representation of the driving force.

Resolving intragranular stress fields in plastically deformed titanium using point-focused high-energy diffraction microscopy

The response of a polycrystalline material to a mechanical load depends not only on the response of each individual grain, but also on the interaction with its neighbors. These interactions lead to local, intragranular stress concentrations that often dictate the initiation of plastic deformation and consequently the macroscopic stress–strain behavior. However, very few experimental studies have quantified intragranular stresses across bulk, three-dimensional volumes. In this work, a synchrotron X-ray diffraction technique called point-focused high-energy diffraction microscopy (pf-HEDM) is used to characterize intragranular deformation across a bulk, plastically deformed, polycrystalline titanium specimen. The results reveal the heterogenous stress distributions within individual grains and across grain boundaries, a stress concentration between a low and high Schmid factor grain pair, and a stress gradient near an extension twinning boundary. This work demonstrates the potential for the future use of pf-HEDM for understanding the local deformation associated with networks of grains and informing mesoscale models.Graphical abstract

FAIR principles for AI models with a practical application for accelerated high energy diffraction microscopy

A concise and measurable set of FAIR (Findable, Accessible, Interoperable and Reusable) principles for scientific data is transforming the state-of-practice for data management and stewardship, supporting and enabling discovery and innovation. Learning from this initiative, and acknowledging the impact of artificial intelligence (AI) in the practice of science and engineering, we introduce a set of practical, concise, and measurable FAIR principles for AI models. We showcase how to create and share FAIR data and AI models within a unified computational framework combining the following elements: the Advanced Photon Source at Argonne National Laboratory, the Materials Data Facility, the Data and Learning Hub for Science, and funcX, and the Argonne Leadership Computing Facility (ALCF), in particular the ThetaGPU supercomputer and the SambaNova DataScale® system at the ALCF AI Testbed. We describe how this domain-agnostic computational framework may be harnessed to enable autonomous AI-driven discovery.

Polymorphism of garnet solid electrolytes and its implications for grain-level chemo-mechanics.

Understanding and mitigating filament formation, short-circuit and solid electrolyte fracture is necessary for advanced all-solid-state batteries. Here, we employ a coupled far-field high-energy diffraction microscopy and tomography approach for assessing the chemo-mechanical behaviour for dense, polycrystalline garnet (Li7La3Zr2O12) solid electrolytes with grain-level resolution. In situ monitoring of grain-level stress responses reveals that the failure mechanism is stochastic and affected by local microstructural heterogeneity. Coupling high-energy X-ray diffraction and far-field high-energy diffraction microscopy measurements reveals the presence of phase heterogeneity that can alter local chemo-mechanics within the bulk solid electrolyte. These local regions are proposed to be regions with the presence of a cubic polymorph of LLZO, potentially arising from local dopant concentration variation. The coupled tomography and FF-HEDM experiments are combined with transport and mechanics modelling to illustrate the degradation of polycrystalline garnet solid electrolytes. The results showcase the pathways for processing high-performing solid-state batteries.

3D In-situ Stop Action Study of Recrystallization in Additively Manufactured 316L Stainless Steel: Reconstruction Optimization and Observations

A volume of an additively manufactured 316L stainless steel sample has been tracked during its recrystallization using near- and far-field High Energy Diffraction Microscopy (HEDM) and absorption tomography at Advanced Photon Source beamline 1-ID. A near-field compatible in situ furnace allows monitoring of Bragg diffraction signals as they evolve out of a weak and diffuse background while the sample temperature is ≈ 1250° C. The sample is rapidly cooled to room temperature after observation of significant signal evolution and ∼ 0.035 mm3 is mapped by the near-field method. Four cycles of heat treatment follow the structure from a state of small, isolated grains through impingement of domains to near completion of recyrstallization. Here, the experiment and reconstructions are described, and recrystallized fractions, twin domains, and distributions of grain boundary types are discussed.

The dynamics of recrystallized grains during static recrystallization in a hot-compressed Mg-3.2Zn-0.1Ca wt.% alloy using in-situ far field high-energy diffraction microscopy

The poor formability of rolled magnesium (Mg) alloy sheet remains a barrier to its widespread commercial use and is attributed to the strong basal texture that occurs in most mechanically processed Mg alloys. Recent attempts to successfully weaken the texture have been made using Mg-Zn-Ca alloys in combination with post-deformation annealing. The motivation for this work is to understand the evolution of the mesoscale processes that occur during annealing (specifically, static recrystallization) and lead to this texture weakening. Toward this goal, more than 1,200 recrystallized grains were studied during in-situ annealing in an 80% hot-compressed Mg-3.2Zn-0.1Ca wt.% (ZX30) alloy using far-field high-energy diffraction (ff-HEDM). The relative volume, crystallographic orientation, and position of each recrystallized grain emerging within a 1 × 1 × 0.1 mm3vol were tracked throughout static recrystallization. These measurements were used to quantitatively measure the nucleation and growth statistics associated with recrystallized grains as a function of annealing time. The measurements reflected a highly heterogeneous process with individual grain dynamics varying wildly from the average, and they also point to relations between relative grain volume and growth rate (or more accurately, the rate of change of volume) with a peak average rate occurring early in recrystallization (at 22% recrystallized). We also explore whether a recrystallized grain's current state can be used to predict its future growth behaviors with implications for Monte Carlo simulations. Finally, we investigate whether recrystallized grains with specific orientations have preferential nucleation and/or growth, and we find that grains with a weak basal texture have a pronounced nucleation advantage that increases with annealing time, while other grain orientations have a slight growth advantage that diminishes with annealing time.

BraggNN: fast X-ray Bragg peak analysis using deep learning.

X-ray diffraction based microscopy techniques such as high-energy diffraction microscopy (HEDM) rely on knowledge of the position of diffraction peaks with high precision. These positions are typically computed by fitting the observed intensities in detector data to a theoretical peak shape such as pseudo-Voigt. As experiments become more complex and detector technologies evolve, the computational cost of such peak-shape fitting becomes the biggest hurdle to the rapid analysis required for real-time feedback in experiments. To this end, we propose BraggNN, a deep-learning based method that can determine peak positions much more rapidly than conventional pseudo-Voigt peak fitting. When applied to a test dataset, peak center-of-mass positions obtained from BraggNN deviate less than 0.29 and 0.57 pixels for 75 and 95% of the peaks, respectively, from positions obtained using conventional pseudo-Voigt fitting (Euclidean distance). When applied to a real experimental dataset and using grain positions from near-field HEDM reconstruction as ground-truth, grain positions using BraggNN result in 15% smaller errors compared with those calculated using pseudo-Voigt. Recent advances in deep-learning method implementations and special-purpose model inference accelerators allow BraggNN to deliver enormous performance improvements relative to the conventional method, running, for example, more than 200 times faster on a consumer-class GPU card with out-of-the-box software.

Chemoheteroepitaxy of 3C‐SiC(111) on Si(111): Influence of Predeposited Ge on Structure and Composition

Secondary ion mass spectroscopy, Fourier transformed infrared spectroscopy, ellipsometry, reflection high energy diffraction and transmission electron microscopy are used to gain inside into the effect of Ge on the formation of ultrathin 3C‐SiC layers on Si(111) substrates. Accompanying the experimental investigations with simulations it is found that the ultrathin single crystalline 3C‐SiC layer is formed on top of a gradient Si1–x–yGexCy buffer layer due to a complex alloying and alloy decomposition processes promoted by carbon and germanium interdiffusion and SiC nucleation. This approach allows tuning residual stress at very early growth stages as well as the interface properties of the 3C‐SiC/Si heterostructure. Useful yields of secondary ions of Ge in Si matrix and Si dimer are estimated.

Formation of Dislocations and Stacking Faults in Embedded Individual Grains during In Situ Tensile Loading of an Austenitic Stainless Steel.

The formation of stacking faults and dislocations in individual austenite (fcc) grains embedded in a polycrystalline bulk Fe-18Cr-10.5Ni (wt.%) steel was investigated by non-destructive high-energy diffraction microscopy (HEDM) and line profile analysis. The broadening and position of intensity, diffracted from individual grains, were followed during in situ tensile loading up to 0.09 strain. Furthermore, the predominant deformation mechanism of the individual grains as a function of grain orientation was investigated, and the formation of stacking faults was quantified. Grains oriented with [100] along the tensile axis form dislocations at low strains, whilst at higher strains, the formation of stacking faults becomes the dominant deformation mechanism. In contrast, grains oriented with [111] along the tensile axis deform mainly through the formation and slip of dislocations at all strain states. However, the present study also reveals that grain orientation is not sufficient to predict the deformation characteristics of single grains in polycrystalline bulk materials. This is witnessed specifically within one grain oriented with [111] along the tensile axis that deforms through the generation of stacking faults. The reason for this behavior is due to other grain-specific parameters, such as size and local neighborhood.

Repeatability and sensitivity characterization of the far-field high-energy diffraction microscopy instrument at the Advanced Photon Source.

In the last two decades, far-field high-energy diffraction microscopy (FF-HEDM) and similar non-destructive techniques have been actively developed at synchrotron light sources around the world. As these techniques (and associated analysis tools) are becoming more available for the general users of these light sources, it is important and timely to characterize their performance and capabilities. In this work, the FF-HEDM instrument implemented at the 1-ID-E endstation of the Advanced Photon Source (APS) is summarized. The set of measurements conducted to characterize the instrument's repeatability and sensitivity to changes in grain orientation and position are also described. When an appropriate grain matching method is used, the FF-HEDM instrument's repeatability is approximately 5 µm in translation, 0.02° in rotation, and 2 × 10-4 in strain; the instrument sensitivity is approximately 5 µm in translation and 0.05° in rotation.

Epitaxial re-solidification of laser-melted Ni-Mn-Ga single crystal

Additive manufacturing (AM) of magnetic shape-memory alloys (MSMAs) allows fuller use of geometry in the design of MSMA parts and avoids the segregation and high cost associated with single crystal production. While most research effort in AM of MSMAs pursues functional foams or polycrystals, epitaxial growth during liquid-phase AM may enable fully-dense single-crystalline MSMA parts, with associated availability of the full blocking stress. We melted a Ni51Mn24.4Ga24.6 single crystal with a moving laser spot under several process parameter combinations of laser power and velocity. While tracks created with lower laser travel velocity were almost entirely epitaxial, the track created with highest velocity (10 mm/s) included non-epitaxial columnar grains and grains at the top of the track. Synchrotron-based high-energy diffraction microscopy (HEDM) experiments revealed that mosaic spread of epitaxial material was slightly higher than that of surrounding non-re-solidified material. Our results demonstrate epitaxial growth of Ni-Mn-Ga with minimal grain content using full-melting laser processing.