Recent breakthroughs in high energy density (HED) science, the study of materials at extreme conditions of pressure and temperature, are profoundly reshaping our understanding across multiple scientific fields. HED science encompasses extreme states of matter across plasma physics, warm dense matter, and condensed matter, bridging fields such as planetary science, materials science, and fusion energy research. Enabled by revolutionary technologies such as ultraintense laser-driven compression, novel insights are emerging from continuous developments. Historically anchored in plasma science, HED physics is evolving toward the understanding of new states of matter, following technological advances. In this Essay, I will present my view of HED science, with particular emphasis on a relatively new and unexplored area within the field that extends beyond plasma physics and warm dense matter, and includes condensed solid and liquid matter at extreme densities and (relatively) cold temperatures. Part of a series of Essays which concisely present author visions for the future of their field.
Powder x-ray diffraction (PXRD) under laser-driven dynamic compression is a powerful tool to investigate material response to extreme pressure, temperature and strain rates. Robust PXRD platforms have been developed at kJ and MJ laser facilities worldwide including the Powder X-Ray Diffraction Image Plate (PXRDIP) at the Omega Laser Facility at the Laboratory for Laser Energetics (LLE) and the TARget Diffraction In Situ (TARDIS) at the National Ignition Facility (NIF). Here we present further developments of data analysis methods focused towards improving the fidelity of the PXRD intensity determination for these platforms. We illustrate these methods by discussing how they can be implemented in a data analysis package and applied to shock compression data on diamond near 1 TPa. We discuss using the XRD signal from the collimating pinhole or a layer of un-compressed material in the sample package as in-situ references for XRD intensity. We detail how to compare data collected with different x-ray sources and how to account for thermal damping of XRD signal when comparing XRD from a shock-compressed, hot material with the reference material at ambient.
Carbon’s abundance, strong covalent bonding and relevance to inertial confinement fusion and planetary science have motivated extensive investigation of its phase diagram at terapascal pressures. However, the melting curve and the existence of phases beyond diamond remain uncertain. Here we resolve the discrepancy between experiments and theoretical simulations of the melting temperature of diamond and show that the diamond structure persists up to 1 TPa. This contradicts a previous report of a transition to the BC8 phase, which density functional theory predicts to be the thermodynamically stable phase of carbon above pressures around 1 TPa. We combine optical velocimetry, pyrometry and X-ray diffraction to probe microcrystalline diamond under nanosecond shock compression. Shock temperature and reflectivity measurements reveal changes in thermodynamic and optical properties, along with a decrease in X-ray diffraction intensity. These results provide evidence for shock-induced melting with a slight decrease in melting temperature with increasing pressure near 7,300 K. Our work delivers atomic-scale benchmarks for quantum simulations of condensed matter at extreme conditions, with implications for planetary interiors. Our improved understanding of diamond melting might also be relevant for achieving higher energy gain in laser-driven nuclear fusion. The location of the melting curve of diamond is unclear. Now, this is illuminated with shock compression experiments that provide strong evidence for shock-induced melting.
This roadmap presents the state-of-the-art, current challenges and near future developments anticipated in the thriving field of warm dense matter physics. Originating from strongly coupled plasma physics, high pressure physics and high energy density science, the warm dense matter physics community has recently taken a giant leap forward. This is due to spectacular developments in laser technology, diagnostic capabilities, and computer simulation techniques. Only in the last decade has it become possible to perform accurate enough simulations & experiments to truly verify theoretical results as well as to reliably design experiments based on predictions. Consequently, this roadmap discusses recent developments and contemporary challenges that are faced by theoretical methods, and experimental techniques needed to create and diagnose warm dense matter. A large part of this roadmap is dedicated to specific warm dense matter systems and applications in astrophysics, inertial confinement fusion and novel material synthesis.
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.
High-energy-density laser facilities and advances in dynamic compression techniques have expanded access to material states in the Terapascal regime relevant to inertial confinement fusion, planetary science, and geophysics. However, experimentally determining the material temperature in these extreme conditions has remained a difficult challenge. Extended X-ray Absorption Fine Structure (EXAFS), referring to the modulations in x-ray absorption above an absorption edge from photoelectrons’ interactions with neighboring atoms, has proven to be a versatile and robust technique for probing material temperature and density for mid-to-high Z elements under dynamic compression. The current platform at the National Ignition Facility has developed six configurations for EXAFS measurements between 7 and 18 keV for different absorption edges (Fe K, Co K, Cu K, Ta L3, Pb L3, and Zr K) using a curved-crystal spectrometer and a bright, continuum foil x-ray source. In this work, we describe the platform geometry, x-ray source performance, spectrometer resolution and throughput, design considerations, and data in ambient and dynamic-compression conditions.
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.
Experiments today can compress solids near isentropically to pressures approaching 100 × 106 atmospheres; however, determining the temperature of such matter remains a major challenge. Extended x-ray absorption fine-structure (EXAFS) spectroscopy is one of the few techniques sensitive to the bulk temperature of highly compressed solid matter, and the validity of this temperature measurement relies on constraining the local ion structure from the EXAFS spectrum. At high-energy-density (HED) conditions, the local ion structure often becomes distorted, which must be accounted for during the EXAFS analysis. Described here is a technique, using a parametrized ion-distribution model to directly analyze EXAFS spectra that provides a better constraint on the local structure than traditional second- or third-order cumulant expansion techniques at HED conditions. The parametrized ion-distribution model is benchmarked by analyzing EXAFS spectra from nickel molecular-dynamics simulations at ∼100 GPa and shown to provide a 10%–20% improvement in constraining the cumulants of the true ion distribution.
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.
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.
Two extended x-ray absorption fine structure flat crystal x-ray spectrometers (EFX's) were designed and built for high-resolution x-ray spectroscopy over a large energy range with flexible, on-shot energy dispersion calibration capabilities. The EFX uses a flat silicon [111] crystal in the reflection geometry as the energy dispersive optic covering the energy range of 6.3-11.4 keV and achieving a spectral resolution of 4.5 eV with a source size of 50 μm at 7.2 keV. A shot-to-shot configurable calibration filter pack and Bayesian inference routine were used to constrain the energy dispersion relation to within ±3 eV. The EFX was primarily designed for x-ray absorption fine structure (XAFS) spectroscopy and provides significant improvement to the Laboratory for Laser Energetics' OMEGA-60 XAFS experimental platform. The EFX is capable of performing extended XAFS measurements of multiple absorption edges simultaneously on metal alloys and x-ray absorption near-edge spectroscopy to measure the electron structure of compressed 3d transition metals.
Large laser facilities have recently enabled material characterization at the pressures of Earth and Super-Earth cores. However, the temperature of the compressed materials has been largely unknown, or solely relied on models and simulations, due to lack of diagnostics under these challenging conditions. Here, we report on temperature, density, pressure, and local structure of copper determined from extended x-ray absorption fine structure and velocimetry up to 1 Terapascal. These results nearly double the highest pressure at which extended x-ray absorption fine structure has been reported in any material. In this work, the copper temperature is unexpectedly found to be much higher than predicted when adjacent to diamond layer(s), demonstrating the important influence of the sample environment on the thermal state of materials; this effect may introduce additional temperature uncertainties in some previous experiments using diamond and provides new guidance for future experimental design.
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.
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.
Most experimentally known high-pressure ice phases have a body-centred cubic (bcc) oxygen lattice. Our large-scale molecular-dynamics simulations with a machine-learning potential indicate that, amongst these bcc ice phases, ices VII, VII′ and X are the same thermodynamic phase under different conditions, whereas superionic ice VII″ has a first-order phase boundary with ice VII′. Moreover, at about 300 GPa, the transformation between ice X and the P bcm phase has a sharp structural change but no apparent activation barrier, whilst at higher pressures the barrier gradually increases. Our study thus clarifies the phase behaviour of the high-pressure ices and reveals peculiar solid–solid transition mechanisms not known in other systems.