Ashley Bucsek

The scientific motivation for this Long-Term Proposal (LTP) is to use in-situ dark-field X-ray microscopy (DFXM) to develop fundamental understanding and predictive capability for the coexisting pathways of different deformation mechanisms in materials essential to next-generation low-carbon technologies when subject to coupled sample environments. This LTP will focus on metallic materials for hydrogen aircraft propulsion systems, lightweight automotive structures, and solid-state aerospace actuators. The developmental goal is to develop a versatile sample environment for in-situ DFXM at the European Synchrotron Radiation Facility’s Extremely Brilliant Source (ESRF-EBS) flagship beamline ID03. The product will be a versatile coupled sample environment that resides on ID03 so that the DFXM user community can utilize it for scientific cases including but not limited to thermomechanical behavior, hydrogen embrittlement, fatigue, and stress-assisted corrosion.

This study investigates the mechanics of prismatic and first-order pyramidal 〈 a 〉 slip in titanium (Ti), elucidating the physics of easy-glide and cross-slip through a combination of theory and experiments. Screw-character prismatic (Pr) dislocations in Ti are of particular interest because their complex cores can be stable or unstable, leading to activation by either cross-slip or planar glide. To investigate these mechanisms, site-specific micro tensile samples were prepared using focused ion beam (FIB) milling and mounted on a push-to-pull (PTP) device for in-situ transmission electron microscopy (TEM) tensile testing. The in-situ experiments provide direct observations of the onset of dislocation motion and the precise determination of the critical resolved shear stress (CRSS) for the activated mechanisms, and its evolution with load cycling. A comprehensive theory has been developed to predict the CRSS values for easy glide, cross-slip, and multiplication of dislocations. Predicted critical stresses for pyramidal (π)-to-Pr and reverse cross-slip agree closely with the experimental measurements. The latter cross-slip stress is a factor of two higher than that of unobstructed planar slip. The model accounts for overlapping dislocation cores and employs a Wigner-Seitz based cell to evaluate misfit energies. By combining ab initio density functional theory (DFT) with anisotropic elasticity, the framework identifies minimum energy pathways for dislocation glide, which can be intermittent and zig-zag. A simplified expression utilizing (π) and Pr Schmid factor ratios is proposed for critical stress corresponding to (π)-to-Pr cross-slip transition. The results are strongly dependent on crystal orientation, underscoring non-Schmid behavior. Overall, this study explores key critical stress parameters essential for informing higher-scale simulations of plasticity in Ti.

Wide bandgap semiconductors with high room temperature mobilities are promising materials for high-power electronics. Stannate films provide wide bandgaps and optical transparency, although electron–phonon scattering can limit mobilities. In SrSnO 3, epitaxial strain engineering stabilizes a high-mobility tetragonal phase at room temperature, resulting in a 3-fold increase in electron mobility among doped films. However, strain relaxation in thicker films leads to nanotextured coexistence of tetragonal and orthorhombic phases with unclear implications for optoelectronic performance. The observed nanoscale phase coexistence demands nanospectroscopy to supply spatial resolution beyond conventional, diffraction-limited microscopy. With nanoinfrared spectroscopy, we provide a comprehensive analysis of phase coexistence in SrSnO 3 over a broad energy range, distinguishing inhomogeneous phonon and plasma responses arising from structural and electronic domains. We establish Nanoscale Imaging and Spectroscopy with Machine-learning Assistance (NISMA) to map nanotextured phases and quantify their distinct optical responses through a robust quantitative analysis, which can be applied to a broad array of complex oxide materials.

Far-field high-energy diffraction microscopy (ff-HEDM) bridges a critical gap between microscale and macroscale plasticity by enabling three-dimensional (3D) time-resolved observations of grain-scale deformation. It can be used to measure the grain-averaged elastic strain tensor, crystallographic orientation, centroid and relative volume of each individual grain. Researchers have also proposed methods to extract information about grain-scale plastic deformation from time-resolved ff-HEDM measurements, using e.g. signature changes in a grain's equivalent or resolved shear stress, orientation or diffraction peak width. However, the accuracy of these different methods is largely unexplored due to the absence of an independent ground truth, particularly for plastic deformation that occurs prior to the macroscopic yield point. In the present work, we evaluate four methods for detecting grain-scale plastic deformation events using ff-HEDM: (i) equivalent stress relaxation, (ii) resolved shear stress relaxation, (iii) orientation change and (iv) diffraction peak shape evolution. Using ff-HEDM data from room-temperature creep tests of a Ti–7Al alloy, we cross-validate these approaches. The achieved high validation rates support confidence in the identified events. Two types of stress relaxation are observed among the detected events – fast and large versus gradual and small – suggesting different deformation mechanisms. The spatiotemporal distribution of plastic events is also captured, revealing clustered activity and intergranular propagation. These findings open avenues for future studies to explore the initiation and propagation of plasticity among grains.

The design of structural&functional materials for specialized applications is being fueled by rapid advancements in materials synthesis, characterization, manufacturing, with sophisticated computational materials modeling frameworks that span a wide spectrum of length&time scales in the mesoscale between atomistic&continuum approaches. This is leading towards a systems-based design methodology that will replace traditional empirical approaches, embracing the principles of the Materials Genome Initiative. However, several gaps remain in this framework as it relates to advanced structural materials:(1) limited availability&access to high-fidelity experimental&computational datasets, (2) lack of co-design of experiments&simulation aimed at computational model validation,(3) lack of on-demand access to verified and validated codes for simulation and for experimental analyses,&(4) limited opportunities for workforce training and educational outreach. These shortcomings stifle major innovations in structural materials design. This paper describes plans for a community-driven research initiative that addresses current gaps based on best-practice recommendations of leaders in mesoscale modeling, experimentation&cyberinfrastructure obtained at an NSF-sponsored workshop dedicated to this topic. The proposal is to create a hub for Mesoscale Experimentation and Simulation co-Operation (hMESO)-that will (I) provide curation and sharing of models, data,&codes, (II) foster co-design of experiments for model validation with systematic uncertainty quantification,&(III) provide a platform for education&workforce development. It will engage experimental&computational experts in mesoscale mechanics and plasticity, along with mathematicians and computer scientists with expertise in algorithms, data science, machine learning,&large-scale cyberinfrastructure initiatives.

At two-thirds the weight of aluminum, magnesium alloys have the potential to reduce the fuel consumption of transportation vehicles. These advancements depend on our ability to optimize the desirable versus undesirable effects of deformation twins, which are three-dimensional (3D) microstructural domains that form under mechanical stresses. Previously only characterized through surface or thin-film measurements, we present 3D in situ characterization of deformation twinning inside an embedded grain over mesoscopic fields of view using dark-field x-ray microscopy supported by crystal plasticity finite element analysis. The results revealed the role of triple junctions on twin nucleation and the sequence and irregularity of twin growth and showed that twin-grain junctions, twin-twin junctions, and twin boundaries were the sites of localized dislocation accumulation.

Wide bandgap semiconductors with high room temperature mobilities are promising materials for high-power electronics. Stannate films provide wide bandgaps and optical transparency, although electron-phonon scattering can limit mobilities. In SrSnO3, epitaxial strain engineering stabilizes a high-mobility tetragonal phase at room temperature, resulting in a threefold increase in electron mobility among doped films. However, strain relaxation in thicker films leads to nanotextured coexistence of tetragonal and orthorhombic phases with unclear implications for optoelectronic performance. The observed nanoscale phase coexistence demands nano-spectroscopy to supply spatial resolution beyond conventional, diffraction-limited microscopy. With nano-infrared spectroscopy, we provide a comprehensive analysis of phase coexistence in SrSnO3 over a broad energy range, distinguishing inhomogeneous phonon and plasma responses arising from structural and electronic domains. We establish Nanoscale Imaging and Spectroscopy with Machine-learning Assistance (NISMA) to map nanotextured phases and quantify their distinct optical responses through a robust quantitative analysis, which can be applied to a broad array of complex oxide materials.

Abstract In this study, we explored the effect of Zn content on the static recrystallization of three 80 pct hot-compressed alloys, Mg–0.5Zn–0.1Ca wt pct (ZX050), Mg–1Zn–0.1Ca wt pct (ZX10), and Mg–3.2Zn–0.1Ca wt pct (ZX30), using far-field high-energy microscopy (ff-HEDM). Individual recrystallized grains were tracked and their 3D centroid, relative volume, and grain-averaged crystallographic orientation were measured during annealing. These measurements were used to compare the recrystallization kinetics and texture evolution of recrystallized grains in ZX alloys as a function of the Zn content. Fully recrystallized microstructures were observed for the ZX30 and the ZX10 alloys after annealing at 230 °C and 330 °C, respectively. In contrast, only a partially recrystallized microstructure for the ZX050 alloy was observed after > 1 hour of annealing at 430 °C. The resistance to recrystallization with decreasing Zn content was also confirmed by detecting faster growth rates of recrystallized grains in the ZX10 and ZX30 alloys, and slower growth rates in the ZX050 alloy. The significant recrystallization texture weakening of the ZX10 and ZX30 alloys and the development of a basal texture in the ZX05 alloy were described based on the orientation dependency of nucleation and growth of recrystallized grains. The analysis demonstrated that texture weakening was associated with increasing Zn content in Mg–Zn–Ca alloys.

Three-dimensional x-ray diffraction (3DXRD), a rotating x-ray diffraction technique, is a powerful tool for studying the micromechanical behavior of polycrystalline materials, capable of measuring the volume, position, orientation, and strain of thousands of grains simultaneously. However, its application has been historically limited to synchrotron facilities. Here, we present the first demonstration of laboratory-scale 3DXRD (Lab-3DXRD) using a liquid-metal-jet source. Lab-3DXRD achieves accuracy comparable to synchrotron-based 3DXRD, as validated against laboratory diffraction contrast tomography (LabDCT) and synchrotron-3DXRD. Over 96% of the grains detected with Lab-3DXRD are cross-validated, particularly for coarse grains (> ~60 μm), while the results suggest that finer grains should be accessible by taking advantage of high-efficiency detectors. We further demonstrate that its sensitivity to finer grains is enhanced by incorporating pre-characterization into the analysis. This study establishes Lab-3DXRD as a practical alternative to synchrotron techniques, making 3DXRD accessible to a wider range of academic and industrial researchers. 3D x-ray diffraction (3DXRD) is a powerful technique for studying the mechanical behavior of polycrystalline materials. Historically limited to synchrotrons, here, we present the first demonstration of 3DXRD at the laboratory scale (Lab-3DXRD).

The design of structural & functional materials for specialized applications is being fueled by rapid advancements in materials synthesis, characterization, manufacturing, with sophisticated computational materials modeling frameworks that span a wide spectrum of length & time scales in the mesoscale between atomistic & continuum approaches. This is leading towards a systems-based design methodology that will replace traditional empirical approaches, embracing the principles of the Materials Genome Initiative. However, several gaps remain in this framework as it relates to advanced structural materials:(1) limited availability & access to high-fidelity experimental & computational datasets, (2) lack of co-design of experiments & simulation aimed at computational model validation,(3) lack of on-demand access to verified and validated codes for simulation and for experimental analyses, & (4) limited opportunities for workforce training and educational outreach. These shortcomings stifle major innovations in structural materials design. This paper describes plans for a community-driven research initiative that addresses current gaps based on best-practice recommendations of leaders in mesoscale modeling, experimentation & cyberinfrastructure obtained at an NSF-sponsored workshop dedicated to this topic. The proposal is to create a hub for Mesoscale Experimentation and Simulation co-Operation (hMESO)-that will (I) provide curation and sharing of models, data, & codes, (II) foster co-design of experiments for model validation with systematic uncertainty quantification, & (III) provide a platform for education & workforce development. It will engage experimental & computational experts in mesoscale mechanics and plasticity, along with mathematicians and computer scientists with expertise in algorithms, data science, machine learning, & large-scale cyberinfrastructure initiatives.

At two-thirds the weight of aluminum, magnesium alloys have the potential to significantly reduce the fuel consumption of transportation vehicles. These advancements depend on our ability to optimize the desirable versus undesirable effects of deformation twins: three dimensional (3D) microstructural domains that form under mechanical stresses. Previously only characterized using surface or thin-film measurements, here, we present the first 3D in-situ characterization of deformation twinning inside an embedded grain over mesoscopic fields of view using dark-field X-ray microscopy supported by crystal plasticity finite element analysis. The results reveal the important role of triple junctions on twin nucleation, that twin growth behavior is irregular and can occur in several directions simultaneously, and that twin-grain and twin-twin junctions are the sites of localized dislocation accumulation, a necessary precursor to crack initiation.

Abstract Refractory complex concentrated alloys (RCCAs) show potential as the next-generation structural materials due to their superior strength in extreme environments. However, RCCAs processed by metal additive manufacturing (AM) typically suffer from process-related challenges surrounding laser material interaction defects and microstructure control. Multimodal in situ techniques (synchrotron X-ray imaging and diffraction and infrared imaging) and melt pool-level simulations were employed to understand rapid solidification pathways in two representative RCCAs: (i) multi-phase BCC + HCP Ti 0.4 Zr 0.4 Nb 0.1 Ta 0.1 and (ii) single-phase BCC Ti 0.486 V 0.375 Cr 0.111 Ta 0.028 . As expected, laser material interaction defects followed similar systematic trends in process parameter space for both alloys. Additionally, both alloys formed a single-phase (BCC) microstructure after rapid solidification processing. However, significant differences in microstructure selection between these alloys were discovered, where Ti 0.4 Zr 0.4 Nb 0.1 Ta 0.1 showed a mixture of equiaxed and columnar grains, while Ti 0.486 V 0.375 Cr 0.111 Ta 0.028 was dominated by columnar growth. These behaviors were well described by the influence of undercooling effects on columnar-to-equiaxed transition (CET). Distinct microstructure formation in each alloy was verified through CET predictions via analytical melt pool simulations, which showed a ~ 5 × increase degrees in undercooling for Ti 0.4 Zr 0.4 Nb 0.1 Ta 0.1 compared to Ti 0.486 V 0.375 Cr 0.111 Ta 0.028 . Overall, these results show that microstructure control based on modulating the freezing range must be balanced with process considerations which resist defect formation, such as solidification crack formation in RCCAs. Graphical abstract

Abstract Interfacial stress fields play a critical role governing the hysteresis and functional fatigue of shape memory alloys. These stress fields manifest at austenite-martensite interfaces (i.e., habit planes) as a consequence of geometric incompatibility between the austenite and martensite phases. As the material approaches transformation, these interfacial stress fields act as an energy barrier, requiring extra energy to be driven into the system to overcome it, resulting in a hysteresis. In addition, increasing the energy in the system also increases dislocation generation, resulting in functional fatigue. In this research, we employ dark-field X-ray microscopy (DFXM), a high-resolution diffraction microstructure imaging technique, to characterize austenite-martensite interfaces and interfacial stress fields during mechanical cycling in a CuAlNi shape memory alloy. The results show, in 3D, the emergence and evolution of individual austenite-martensite interfaces and spatially mapped orientation and elastic strain, including the interfacial elastic strain fields at austenite-martensite interfaces. These findings will contribute to a better understanding of the origins of hysteresis and functional fatigue by investigating interfacial stress fields and dislocation generation at phase interfaces and their effects on macroscopic behavior.

Abstract The crystallographic theory of martensite (CTM) forms the foundation of our understanding of stress-induced reversible martensitic phase transformation cycling, relying on assumptions that exclude precipitates, grain boundaries, plasticity, and strained lattices. An ongoing challenge persists in adapting our understanding of CTM-based micromechanical theory (e.g., habit plane variant, or HPV, prediction and the origins of hysteresis and, subsequently, functional fatigue) to real, engineering-grade SMAs. Due to the complexity, elucidating the micromechanical phenomena requires novel high-resolution 3D in-situ characterization techniques.

The determination of Critical Resolved Shear Stress (CRSS) in titanium for basal, prismatic, and pyramidal slip-planes without empirical constants is presented by combining Density Functional Theory (DFT) and anisotropic elasticity. A new mechanism leading to tension-compression (T-C) asymmetry in the CRSS levels has been revealed for the first time. The conditions for this asymmetry are established, involving a complex interplay between the dislocation core-structure and core-advance behavior. The three conditions for T-C asymmetry that need to be simultaneously satisfied can be summarized as: (1) a medium stacking fault width, d, (3<d/bF<10, where bF is the magnitude of the Burgers vector of the full dislocation), (2) an asymmetric core-structure of the extended dislocation (ξ1≠ξ2, where ξ1 and ξ2 are the core-widths of the first and second partials, respectively), and (3) intermittent motion of the partials (Δd/bF≠0, where Δd is the magnitude of fluctuation in stacking fault width during intermittent motion). Pyramidal-slip in titanium satisfies all three conditions, resulting in significant T-C asymmetry. The CRSS theory considers a Wigner-Seitz (W-S) cell based domain area assigned to each lattice site for the calculations of core-energies accurately capturing the slip-plane lattice. The W-S based approach is essential due to the lower symmetry of the HCP crystal circumventing potential errors associated with the one-dimensional atomic-row approximation. Dislocation core structures are obtained for all the slip-systems in titanium showing significant distortion of the disregistry profile governing the core-advance behavior. The CRSS values predicted from the theory show agreement with the experimental CRSS levels reported in the literature.

Abstract Martensite, α‘, commonly appears in Ti-6Al-4V upon rapid cooling from above the β-transus temperature. It is known that α‘ decomposes into α and β at high temperatures but well below the β-transus temperature. Here, we study the decomposition of martensitic Ti-6Al-4V under rapid laser heating, employing in situ synchrotron X-ray diffraction. A comparison is made with post-annealed Ti-6Al-4V under heating to elucidate changes without martensite decomposition. The fast acquisition of X-ray diffraction data at 250 Hz temporally resolves the decomposition process initiated by annihilating dislocations in α‘. The recovery process is accompanied by structural changes in martensite, followed by the phase transformation to β. Thermal profiles estimated from the lattice parameter data reveal the influence of heating rates and dislocation densities on the decomposition process. Throughout the analysis of the diffraction profiles with respect to estimated temperature, we propose a straightforward method for approximating the initiation temperature of martensite decomposition.

Dark-field X-ray microscopy (DFXM) is a high-resolution, X-ray-based diffraction microstructure imaging technique that uses an objective lens aligned with the diffracted beam to magnify a single Bragg reflection. DFXM can be used to spatially resolve local variations in elastic strain and orientation inside embedded crystals with high spatial (~ 60 nm) and angular (~ 0.001°) resolution. However, as with many high-resolution imaging techniques, there is a trade-off between resolution and field of view, and it is often desirable to enrich DFXM observations by combining it with a larger field-of-view technique. Here, we combine DFXM with high-resolution X-ray diffraction (HR-XRD) applied to an in-situ investigation of static recrystallization in an 80% hot-compressed Mg-3.2Zn-0.1Ca wt.% (ZX30) alloy. Using HR-XRD, we track the relative grain volume of > 8000 sub-surface grains during annealing in situ. Then, at several points during the annealing process, we "zoom in" to individual grains using DFXM. This combination of HR-XRD and DFXM enables multiscale characterization, used here to study why particular grains grow to consume a large volume fraction of the annealed microstructure. This technique pairing is particularly useful for small and/or highly deformed grains that are often difficult to resolve using more standard diffraction microstructure imaging techniques.

Abstract 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