For more than a century, x rays have been an essential tool in physics, chemistry, biology, materials science, and other subjects, considerably expanding our understanding of the fundamental structure of materials. X rays and electrons are among the most useful tools in the scientific toolbox for understanding the properties and functions of materials and molecules because of their capacity to penetrate matter and differentiate the structural changes at the atomic level. This information has a wide range of applications, including the development of innovative materials for electronics and clean energy technologies, as well as more effective pharmaceuticals with fewer side effects. A major new field in x-ray science has been opened by recent developments in ultrafast x-ray sources operating in the femtosecond (fs) to atto-second regimes. These advancements make possible element-specific probing of dynamics of charge particles and electronic configurations of electronic motions at fundamental timescales, sensitive probing of structural dynamics in materials at the atomic and electronic level at fundamental timescales, and efficient new methods for examining the coupling between atomic and electronic structural dynamics to investigate the material properties and functions. The most significant advancement has been the latest discovery of x-ray free-electron lasers (XFELs), of which there are now many new facilities either operational or under development worldwide. In addition, the development of high-order harmonic extreme ultraviolet sources based on lasers that operate in the atto-second regime as well as the tabletop and synchrotron-based laser-plasma x-ray sources that operate in the fs regime complement the achievements of XFEL. The current article provides a comprehensive discussion and future perspectives on the application of ultrafast XFELs to study the structure of matter under shock compression.

X-ray free electron laser (XFEL) sources coupled to high-power laser systems offer an avenue to study the structural dynamics of materials at extreme pressures and temperatures. The recent commissioning of the DiPOLE 100-X laser on the high energy density (HED) instrument at the European XFEL represents the state-of-the-art in combining x-ray diffraction with laser compression, allowing for compressed materials to be probed in unprecedented detail. Here, we report quantitative structural measurements of molten Sn compressed to 85(5) GPa and ∼3500 K. The capabilities of the HED instrument enable liquid density measurements with an uncertainty of ∼1% at conditions which are extremely challenging to reach via static compression methods. We discuss best practices for conducting liquid diffraction dynamic compression experiments and the necessary intensity corrections which allow for accurate quantitative analysis. We also provide a polyimide ablation pressure vs input laser energy for the DiPOLE 100-X drive laser which will serve future users of the HED instrument.

The prototypical α→ω phase transition in zirconium is an ideal test bed for our understanding of polymorphism under extreme loading conditions. After half a century of study, a consensus had emerged that the transition is realized via one of two distinct displacive mechanisms, depending on the nature of the compression path. However, recent dynamic-compression experiments equipped with diffraction diagnostics performed in the past few years have revealed new transition mechanisms, demonstrating that our understanding of the underlying atomistic dynamics and transition kinetics is in fact far from complete. We present classical molecular dynamics simulations of the α→ω phase transition in single-crystal zirconium shock compressed along the [0001] axis using a machine-learning-class potential. The transition is predicted to proceed primarily via a modified version of the two-stage Usikov-Zilberstein mechanism, whereby the high-pressure ω phase heterogeneously nucleates at boundaries between grains of an intermediate β phase. We further observe the fomentation of atomistic disorder at the junctions between β grains, leading to the formation of highly defective interstitial material between the ω grains. We directly compare synthetic x-ray diffraction patterns generated from our simulations with those obtained using femtosecond diffraction in recent dynamic-compression experiments, and show that the simulations produce the same unique, anisotropic diffuse scattering signal unlike any previously seen from an elemental metal. Our simulations suggest that the diffuse signal arises from a combination of thermal diffuse scattering, nanoparticlelike scattering from residual kinetically stabilized α and β grains, and scattering from interstitial defective structures. Published by the American Physical Society 2024

On December 5, 2022, an indirect drive fusion implosion on the National Ignition Facility (NIF) achieved a target gain G_{target} of 1.5. This is the first laboratory demonstration of exceeding "scientific breakeven" (or G_{target}>1) where 2.05 MJ of 351 nm laser light produced 3.1 MJ of total fusion yield, a result which significantly exceeds the Lawson criterion for fusion ignition as reported in a previous NIF implosion [H. Abu-Shawareb et al. (Indirect Drive ICF Collaboration), Phys. Rev. Lett. 129, 075001 (2022)PRLTAO0031-900710.1103/PhysRevLett.129.075001]. This achievement is the culmination of more than five decades of research and gives proof that laboratory fusion, based on fundamental physics principles, is possible. This Letter reports on the target, laser, design, and experimental advancements that led to this result.

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.

Laser-driven shock compression enables an experimental study of phase transitions at unprecedented pressures and temperatures. One example is the shock Hugoniot of magnesium oxide (MgO), which crosses the B1-B2-liquid triple point at 400-600 GPa, 10 000-13 000 K (0.86-1.12 eV). MgO is a major component within the mantles of terrestrial planets and has long been a focus of high-pressure research. Here, we combine time-resolved velocimetry and pyrometry measurements with a decaying shock platform to obtain pressure-temperature data on MgO from 300 to 1500 GPa and 9000 to 50 000 K. Pressure-temperature-density Hugoniot data are reported at 1500 GPa. These data represent the near-instantaneous response of an MgO [100] single crystal to shock compression. We report on a prominent temperature anomaly between 400 and 460 GPa, in general agreement with previous shock studies, and draw comparison with equation-of-state models. We provide a detailed analysis of the decaying shock compression platform, including a treatment of a pressure-dependent optical depth near the shock front. We show that if the optical depth of the shocked material is larger than 1 mu m, treating the shock front as an optically thick gray body will lead to a noticeable overestimation of the shock temperature.

Magnesium oxide (MgO) is a major component of the Earth’s mantle and is expected to play a similar role in the mantles of large rocky exoplanets. At extreme pressures, MgO transitions from the NaCl B 1 crystal structure to a CsCl B 2 structure, which may have implications for exoplanetary deep mantle dynamics. In this study, we constrain the phase diagram of MgO with laser-compression along the shock Hugoniot, with simultaneous measurements of crystal structure, density, pressure, and temperature. We identify the B 1 to B 2 phase transition between 397 and 425 gigapascal (around 9700 kelvin), in agreement with recent theory that accounts for phonon anharmonicity. From 425 to 493 gigapascal, we observe a mixed-phase region of B1 and B2 coexistence. The transformation follows the Watanabe-Tokonami-Morimoto mechanism. Our data are consistent with B 2-liquid coexistence above 500 gigapascal and complete melting at 634 gigapascal. This study bridges the gap between previous theoretical and experimental studies, providing insights into the timescale of this phase transition.

A MHz X-ray diffraction set-up for the investigation of material behaviour under dynamic compression in a diamond anvil cell at intermediate strain rates has been developed at the High Energy Density (HED) instrument at the European XFEL.

Active research is ongoing that investigates the properties of matter under extreme pressure. Such condensed matter is found inside planets at millions of atmospheres and thousands of degrees kelvin. Extreme pressures coupled with high temperatures can also be used to synthesize new materials with advanced properties. This Primer outlines how a new generation of X-ray user facilities are essential to measure the microscopic properties of matter under such conditions, with scattering and absorption methods being the most used. This article explains how extreme thermodynamic states can be achieved, either by dynamic laser shock or static diamond anvil cell compression, and how the high-brilliance X-ray beams produced at synchrotrons and hard X-ray free electron lasers can be utilized to investigate very dense matter with a high level of detail and accuracy at the microscopic level. Cross-fertilization between the static and dynamic communities has led to new approaches, bridging timescales and opening new perspectives to understanding dynamic processes at high pressure. To illustrate this, two examples are highlighted: iron and carbon. Reproducibility issues and some limitations are discussed, ending with an evaluation of future opportunities. Studying materials at high temperature and pressure provides information about phase transitions, with different X-ray probes to characterize material properties. This Primer describes how static and dynamic compression at synchrotrons and X-ray free-electron lasers can be used to reach high temperature, high pressure states and probe matter under extreme conditions.

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.

We report measurements of the compressibility of ramp compressed tantalum to a final stress of 2.3 TPa corresponding to threefold volumetric compression. Using these data, we extended the experimental constraint on the Ta cold compression curve by an order of magnitude in pressure. By combining the resulting data with previous measurements of shock compression and ambient pressure heating, we construct an experimentally bounded and thermodynamically consistent equation of state model for Ta which has 2% uncertainty in pressure at 1 TPa. We therefore propose Ta as an in situ pressure scale for laser-heated static compression experiments which were recently able to reach terapascal pressures and thousands of degrees Kelvin. Our new equation of state of Ta is experimentally constrained at extreme pressures and temperatures relevant to a wide range of planetary interiors and will allow for more accurate comparison between experimental measurements and theory at extreme conditions.

Silicon (Si) exhibits a rich collection of phase transitions under ambient-temperature isothermal and shock compression. This report describes in situ diffraction measurements of ramp-compressed Si between 40 and 389 GPa. Angle-dispersive x-ray scattering reveals that Si assumes an hexagonal close-packed (hcp) structure between 40 and 93 GPa and, at higher pressure, a face-centered cubic structure that persists to at least 389 GPa, the highest pressure for which the crystal structure of Si has been investigated. The range of hcp stability extends to higher pressures and temperatures than predicted by theory.

The high-pressure (HP) behavior of dioxides is of interest due to their extensive polymorphism and role as analogs for SiO_{2}, a phase expected to be important in the deep mantles of Earth and terrestrial exoplanets. Here we report on dynamic ramp compression of quartz-type germanium dioxide GeO_{2} to stresses up to 882 GPa, a higher peak stress than previous studies by a factor of 5. X-ray diffraction data show that HP-PdF_{2}-type GeO_{2} occurs under ramp loading from 154 to 440 GPa, and this phase persists to higher pressure than predicted by theory. Above 440 GPa, we observe evidence for transformation to a new phase of GeO_{2}. Based on the diffraction data, the best candidate for this new phase is the cotunnite-type structure which has been predicted to be a stable phase of GeO_{2} above 300 GPa. The HP-PdF_{2}-type and cotunnite-type structures are important phases in a wide range of AX_{2} compounds, including SiO_{2}, at multihundred GPa stresses. Our results demonstrate that ramp compression can be an effective technique for synthesizing and characterizing such phases in oxides. In addition, we show that pulsed x-ray diffraction under ramp compression can be used to examine lower-symmetry phases in oxide materials.

We combine nanosecond laser shock compression with \emph{in-situ} picosecond X-ray diffraction to provide structural data on iron up to 275 GPa. We constrain the extent of hcp-liquid coexistence, the onset of total melt, and the structure within the liquid phase. Our results indicate that iron, under shock compression, melts completely by 258(8) GPa. A coordination number analysis indicates that iron is a simple liquid at these pressure-temperature conditions. We also perform texture analysis between the ambient body-centered-cubic (bcc) $\alpha$, and the hexagonal-closed-packed (hcp) high-pressure $\epsilon-$phase. We rule out the Rong-Dunlop orientation relationship (OR) between the $\alpha$ and $\epsilon-$phases. However, we cannot distinguish between three other closely related ORs: Burger's, Mao-Bassett-Takahashi, and Potter's OR. The solid-liquid coexistence region is constrained from a melt onset pressure of 225(3) GPa from previously published sound speed measurements and full melt (246.5(1.8)-258(8) GPa) from X-ray diffraction measurements, with an associated maximum latent heat of melting of 623 J/g. This value is lower than recently reported theoretical estimates and suggests that the contribution to the earth's geodynamo energy budget from heat release due to freezing of the inner core is smaller than previously thought. Melt pressures for these nanosecond shock experiments are consistent with gas gun shock experiments that last for microseconds, indicating that the melt transition occurs rapidly.

The extreme response of polycrystalline iron at high pressures and high strain rates is revealed by means of high-power laser pulses. The compression portion of the pulse coupled with x-ray diffraction identifies the expected body-centered cubic (α) to hexagonal close packed (ε) displacive transformation. Upon release, observation shows that the complete reverse transformation takes approximately 8 ns and that the structure returns to its initial microstructural configuration, in a reversible transformation path. This is in good agreement with molecular dynamics (MD) simulations which predict an inverse dependence between transformation time and strain rate. The grain size is reduced from μm to nm range during compression and begins increasing back to the original grain size on decompression. The kinetics of the transition is dictated by heterogenous nucleation as it follows the Johnson-Mehl-Avrami-Kolmogorov equation with the appropriate time exponent of ∼1. This is confirmed by MD simulations which also identify profuse twinning and dislocation generation. The tensile pulse generated upon reflection at the free surface is captured by time-resolved free surface velocity measurements from which a peak tensile stress of 7 GPa is obtained, in stark contrast with its quasi-static value of ∼200 MPa. At these strain rates, the strength of grain interiors, which is determined by twinning and slip exceeds the strength of the boundaries, and failure initiates preferentially in the latter.

This report details the analyses and related uncertainties in measuring longitudinal-stress-density paths in indirect laser-driven ramp equation-of-state (EOS) experiments [Smith et al., Nat. Astron. 2(6), 452-458 (2018); Smith et al., Nature 511(7509), 330-333 (2014); Fratanduono et al., Science 372(6546), 1063-1068 (2021); and Fratanduono et al., Phys. Rev. Lett. 124(1), 015701 (2020)]. Experiments were conducted at the National Ignition Facility (NIF) located at the Lawrence Livermore National Laboratory. The NIF can deliver up to 2 MJ of laser energy over 30 ns and provide the necessary laser power and control to ramp compress materials to TPa pressures (1 TPa = 10 × 106 atmospheres). These data provide low-temperature solid-state EOS data relevant to the extreme conditions found in the deep interiors of giant planets. In these experiments, multi-stepped samples with thicknesses in the range of 40-120 µm experience an initial shock compression followed by a time-dependent ramp compression to peak pressure. Interface velocity measurements from each thickness combine to place a constraint on the Lagrangian sound speed as a function of particle velocity, which in turn allows for the determination of a continuous stress-density path to high levels of compressibility. In this report, we present a detailed description of the experimental techniques and measurement uncertainties and describe how these uncertainties combine to place a final uncertainty in both stress and density. We address the effects of time-dependent deformation and the sensitivity of ramp EOS techniques to the onset of phase transformations.

Alumina (Al 2 O 3 ) is an important ceramic material notable for its compressive strength and hardness. It represents one of the major oxide components of the Earth’s mantle. Static compression experiments have reported evidence for phase transformations from the trigonal α -corundum phase to the orthorhombic Rh 2 O 3 (II)-type structure at ∼90 GPa, and then to the post-perovskite structure at ∼130 GPa, but these phases have yet to be directly observed under shock compression. In this work, we describe laser-driven shock compression experiments on polycrystalline alumina conducted at the Matter in Extreme Conditions endstation of the Linac Coherent Light Source. Ultrafast x-ray pulses (50 fs, 10 12 photons/pulse) were used to probe the atomic-level response at different times during shock propagation and subsequent pressure release. At 107 ± 8 GPa on the Hugoniot, we observe diffraction peaks that match the orthorhombic Rh 2 O 3 (II) phase with a density of 5.16 ± 0.03 g cm −3 . Upon unloading, the material transforms back to the α -corundum structure. Upon release to ambient pressure, densities are lower than predicted assuming isentropic release, indicating additional lattice expansion due to plastic work heating. Using temperature values calculated from density measurements, we provide an estimate of alumina’s strength on release from shock compression.

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.