The response of materials under dynamic compression involves a complex interplay of various deformation mechanisms aimed at relieving shear stresses, yielding a remarkable diversity in material behavior. In this Letter, we utilize femtosecond x-ray diffraction coupled with nanosecond laser compression to reveal an intricate competition between multiple shear-relieving mechanisms within an elemental metal. Our observations in shocked-compressed single-crystal Zr indicate a disorder-mediated shear relaxation at lower pressures. Above the phase-transition pressure, we observe the increasing contribution of structural phase transition in relieving shear stress. We detect not one but three concurrent pathways during the transition from the hcp to a hex-3 structure. These complex dynamics are partially corroborated through multimillion-atom molecular dynamics simulations employing a machine-learned interatomic potential. Our observation of multiple concurrent pathways and disorder during shock compression underscore the far greater intricacies in the dynamic response of metals than previously assumed.

As part of a program to measure phase transition timescales in materials under dynamic compression, we have designed new x-ray imaging diagnostics to record multiple x-ray diffraction measurements during a single laser-driven experiment. Our design places several ns-gated hybrid CMOS (hCMOS) sensors within a few cm of a laser-driven target. The sensors must be protected from an extremely harsh environment, including debris, electromagnetic pulses, and unconverted laser light. Another key challenge is reducing the x-ray background relative to the faint diffraction signal. Building on the success of our predecessor (Target Diffraction In Situ), we implemented a staged approach to platform development. First, we built a demonstration diagnostic (Gated Diffraction Development Diagnostic) with two hCMOS sensors to confirm we could adequately protect them from the harsh environment and also acquire acceptable diffraction data. This allowed the team to quickly assess the risks and address the most significant challenges. We also collected scientifically useful data during development. Leveraging what we learned, we recently developed a much more ambitious instrument (Flexible Imaging Diffraction Diagnostic for Laser Experiments) that can field up to eight hCMOS sensors in a flexible geometry and participate in back-to-back shots at the National Ignition Facility (NIF). The design also allows for future iterations, such as faster hCMOS sensors and an embedded x-ray streak camera. The enhanced capabilities of the new instrument required a much more complex design, and the unexpected issues encountered on the first few shots at NIF remind us that complexity has consequences. Our progress in addressing these challenges is described herein, as is our current focus on improving data quality by reducing x-ray background and quantifying the uncertainties of our diffraction measurements.

The traditional picture of solid-solid phase transformations assumes an ordered parent phase transforms into an ordered daughter phase via a single unique pathway. Zirconium and its prototypical phase transition from hexagonal close-packed (hcp) to simple hexagonal (hex-3) structure has generated considerable controversy over several decades regarding which mechanism mediates the transformation. However, a lack of in situ measurements over the relevant atomistic timescales has hindered our ability to identify the true pathway. In this study, we exploit femtosecond X-ray diffraction coupled with nanosecond laser compression to give unprecedented insights into the complexities of how materials transform at the lattice level. We observe single-crystal zirconium changing from hcp to a hex-3 structure via not one but three competing pathways simultaneously. Concurrently, we also observe a broad diffuse background underlying the sharp Bragg diffraction during the transition. We corroborate our observation of the diffuse signal with multimillion-atom molecular dynamics simulations using a machine-learned interatomic potential. Our study demonstrates that the traditional mechanistic view of transitions may fail for even an elemental metal and that the mechanisms by which materials transform are far more intricate than generally thought.

X-ray diffraction is a powerful measurement technique for determining material properties, and it is now possible to perform these experiments at pressures exceeding 1 TPa [Rygg et al., Rev. Sci. Instrum. 91, 043902 (2020)] at the National Ignition Facility (NIF). The x-ray source for these experiments is the quasi-monochromatic Heα emission from metal foils heated to multi-keV temperatures. A critical aspect for understanding the sample's thermodynamic state is the amount of heating caused by absorption of the probe x-rays. In this work, we characterize the performance of the Ge foil x-ray source over more than 60 NIF x-ray diffraction experiments. We use this information to constrain the level of diffraction sample heating from the x-ray source and discuss the impact on the thermodynamic state.

Carbon is the fourth-most prevalent element in the Universe and essential for all known life. In the elemental form it is found in multiple allotropes, including graphite, diamond and fullerenes, and it has long been predicted that even more structures can exist at pressures greater than those at Earth's core(1-3). Several phases have been predicted to exist in the multi-terapascal regime, which is important for accurate modelling of the interiors of carbon-rich exoplanets(4,5.) By compressing solid carbon to 2 terapascals (20 million atmospheres; more than five times the pressure at Earth's core) using ramp-shaped laser pulses and simultaneously measuring nanosecond-duration time-resolved X-ray diffraction, we found that solid carbon retains the diamond structure far beyond its regime of predicted stability. The results confirm predictions that the strength of the tetrahedral molecular orbital bonds in diamond persists under enormous pressure, resulting in large energy barriers that hinder conversion to more-stable high-pressure allotropes(1,2), just as graphite formation from metastable diamond is kinetically hindered at atmospheric pressure. This work nearly doubles the highest pressure at which X-ray diffraction has been recorded on any material.

The discovery of more than 4500 extrasolar planets has created a need for modeling their interior structure and dynamics. Given the prominence of iron in planetary interiors, we require accurate and precise physical properties at extreme pressure and temperature. A first-order property of iron is its melting point, which is still debated for the conditions of Earth's interior. We used high-energy lasers at the National Ignition Facility and in situ x-ray diffraction to determine the melting point of iron up to 1000 gigapascals, three times the pressure of Earth's inner core. We used this melting curve to determine the length of dynamo action during core solidification to the hexagonal close-packed (hcp) structure. We find that terrestrial exoplanets with four to six times Earth's mass have the longest dynamos, which provide important shielding against cosmic radiation.

High-energy synchrotron x-rays are used to track grain-averaged lattice reorientation and stress-state evolution in Ti–7Al as it is cyclically loaded to 90% of its macroscopic yield stress. This evolution provides clear indication of accumulating plastic strain even though the sample never exceeded the elastic limit. The largest changes in lattice orientation and stress state are observed following the first cycle then evolution continues at a lower rate with subsequent cycles. Variation of the axes about which lattice reorientation occurs is found to be highly dependent on the maximum resolved shear stress and corresponding activation of various families of slip systems.

Investigating how solid matter behaves at enormous pressures, such as those found in the deep interiors of giant planets, is a great experimental challenge. Over the past decade, computational predictions have revealed that compression to terapascal pressures may bring about counter-intuitive changes in the structure and bonding of solids as quantum mechanical forces grow in influence 1 – 6 . Although this behaviour has been observed at modest pressures in the highly compressible light alkali metals 7 , 8 , it has not been established whether it is commonplace among high-pressure solids more broadly. We used shaped laser pulses at the National Ignition Facility to compress elemental Mg up to 1.3 TPa, which is approximately four times the pressure at the Earth’s core. By directly probing the crystal structure using nanosecond-duration X-ray diffraction, we found that Mg changes its crystal structure several times with non-close-packed phases emerging at the highest pressures. Our results demonstrate that phase transformations of extremely condensed matter, previously only accessible through theoretical calculations, can now be experimentally explored.

X-ray computed tomography (CT) systems can produce high resolution images, in which small (sub-millimeter) features can be detected. This requires the X-rays to sufficiently penetrate the object and interact strongly enough to produce measurable attenuation. Low atomic number (low Z), low density objects shielded by high atomic number (high Z) materials result in X-ray reconstructions that lack sufficient contrast to differentiate interior features from noise and reconstruction artifacts. Fast neutron CT offers complementary information to X-rays with superior penetration through high Z shielding and with less severe beam hardening artifacts. However, spatial resolution in X-ray imaging systems is generally superior to that of fast neutron imagers. Here, we quantitatively compare these two complementary modalities to demonstrate the ability to observe small feature locations within two multi-material objects. Quantitative measures include calculation of image gradient at material edges, contrast-to-noise ratio, and F1 score.

Dwell fatigue, the reduction in fatigue life experienced by titanium alloys due to holds at stresses as low as 60% of yield, has been implicated in several uncontained jet engine failures. Dislocation slip has long been observed to be an intermittent, scale-bridging phenomenon, similar to that seen in earthquakes but at the nanoscale, leading to the speculation that large stress bursts might promote the initial opening of a crack. Here we observe such stress bursts at the scale of individual grains in situ, using high energy X-ray diffraction microscopy in Ti–7Al–O alloys. This shows that the detrimental effect of precipitation of ordered Ti 3 Al is to increase the magnitude of rare pri〈 a 〉 and bas〈 a 〉 slip bursts associated with slip localisation. By contrast, the addition of trace O interstitials is beneficial, reducing the magnitude of slip bursts and promoting a higher frequency of smaller events. This is further evidence that the formation of long paths for easy basal plane slip localisation should be avoided when engineering titanium alloys against dwell fatigue.

A finite element framework is developed to resolve the intragranular fields of incompatible deformation generated intrinsically in response to applied deformation, through linear elasticity complemented by the theory of continuous distribution of dislocations and experimental grain-scale observations. Discrete grain-averaged lattice strains, characterized along with grain orientations via X-ray diffraction microscopy, enable high fidelity continuous solutions anchored to measured response and satisfy boundary conditions, mechanical equilibrium, and strain compatibility within a finite element model. A continuous distribution of strain fields in a nickel-based superalloy, evaluated periodically during R = 0 cyclic loading, exposes the fundamental heterogeneity in polycrystalline response which creates locations of high stress gradients and potential sites of failure. Incompatibility is shown to be an effective measure driving the spatial concentration of stress with loading, particularly at twin and high angle grain boundaries. Furthermore, incompatible deformation is shown, through both specific examples and statistically, to be predominantly preserved upon elastic recovery improving our understanding of the history dependence of residual stresses. Positive correlation between residual stress & incompatible deformation and saturation of material response or shakedown in response to cyclic loading is revealed. The scalability of the framework with experiments at multiple length scales are discussed.

The advancement of microstructure-sensitive models for elevated temperature applications requires experimental data at the relevant length scales and usage environments. Towards this goal, we studied the evolution of grain-level strains in a Ni-based superalloy during heating and subsequent loading at elevated temperature. The specimen was heated using two halogen lamps in a furnace designed explicitly for the special load frame used for the synchrotron-based experiment. High energy X-ray diffraction was used to non-destructively characterize the initial 3D microstructure, confirm the temperature of the specimen, and monitor the evolution of grain-level strains, stresses, and orientations through the elastic-plastic transition. The distributions of grain-level normal strains were observed to broaden with elastic loading, whereas elastic-plastic loading led to development of local intergranular “hotspots”, or activation of plastic slip within select grains, that both broaden and skew the grain-level strain distributions. These grain-level strain distributions were fit to a generalized extreme value (GEV) distribution function. The GEV shape parameter is observed to change significantly at the onset of macroscopic plasticity. At the grain scale, more grain reorientation (plasticity) occurred for grains oriented for lower strength-to-stiffness ratios. During the onset of plastic deformation for LSHR at 660∘C load shedding from lower strength-to-stiffness-oriented grains to higher strength-to-stiffness-oriented grains was observed. Additionally, based on the grain-averaged reorientation axis, it was found that LSHR has a preference for activation of multiple slip systems at 660∘C. We conclude with a discussion on the critical need for statistical analysis of such mesoscale data obtained in situ at elevated temperature for the verification/validation of the next generation of microstructure-sensitive models.

Hexagonal metals have anisotropic coefficients of thermal expansion causing grain-level internal stresses during heating. High energy x-ray diffraction microscopy, a non-destructive, in situ, micromechanical and microstructural characterization technique, has been used to determine the anisotropic coefficients of thermal expansion (CTEs) for Ti-7Al. Two samples of polycrystalline $\alpha$-phase Ti-7Al were continuously heated from room temperature to 850 $^\circ$C while far-field HEDM scans were collected. The results showed a change in the ratio of the CTEs in the 'a' and 'c' directions which explains discrepancies found in the literature. The CTE additionally appears to be affected by the dissolution of $\alpha_2$ precipitates. Analysis of the grain-resolved micromechanical data also shows reconfiguration of the grain scale stresses likely due to anisotropic expansion driving crystallographic slip.

Understanding dynamics across phase transformations and the spatial distribution of minerals in the lower mantle is crucial for a comprehensive model of the evolution of the Earth's interior. Using the multigrain crystallography technique (MGC) with synchrotron x-rays at pressures of 30 GPa in a laser-heated diamond anvil cell to study the formation of bridgmanite [(Mg,Fe)SiO3] and ferropericlase [(Mg,Fe)O], we report an interconnected network of a smaller grained ferropericlase, a configuration that has been implicated in slab stagnation and plume deflection in the upper part of the lower mantle. Furthermore, we isolated individual crystal orientations with grain-scale resolution, provide estimates on stress evolutions on the grain scale, and report {110} twinning in an iron-depleted bridgmanite, a mechanism that appears to aid stress relaxation during grain growth and likely contributes to the lack of any appreciable seismic anisotropy in the upper portion of the lower mantle.

We describe 3D characterization of an additively manufactured Inconel 625 nickel-base superalloy specimen conducted during a uniaxial tension test using a suite of nondestructive x-ray techniques. High-energy diffraction microscopy in both near- and far-field modalities are employed in situ to track evolution of the material orientation and stress–strain fields at six points during the mechanical test, and these data streams are registered with micro-computed tomography reconstructions which probe the material density. This data volume was matched to a multi-modal serial sectioning characterization of the specimen taken after loading, described in this article’s companion. Twenty-eight grains which were monitored throughout the experiment were selected to form the basis for AFRL AM Modeling Series Challenge 4, Microscale Structure-to-Properties.

The microstructures of Ti-6Al-4V following laser processing depend primarily on the phase transformation of β to α, but their development is constrained by the rapidly changing temperature in the small fusion zone. In-situ synchrotron X-ray diffraction was utilized to probe the rapid phase evolution in single melt tracks with high angular and temporal resolution. Both fully martensitic and mixed α+α′+β microstructures were confirmed by microscopy. Cooling rates were inferred from the lattice parameter history and complementary thermal simulation. It was found that the threshold cooling rate for fully martensitic transformation is in the range between 2900 and 6500°C/s.