FeO (wüstite), which exhibits complex electronic and structural properties with increasing pressure and temperature, is a key mineralogical phase for understanding deep planetary interiors. However, direct measurements of its spin state at high-pressure and temperature remain challenging in static compression experiments. Here, we employ laser-driven shock compression to extend the FeO principal Hugoniot up to ∼900 GPa and perform in situ X-ray diffraction and X-ray emission spectroscopy up to 250 GPa, probing FeO's crystal structure and spin state. We demonstrate a continuous spin crossover of iron in FeO over a broad pressure range, with the high-spin state persisting beyond Earth's core-mantle boundary (CMB) conditions. These observations provide new experimental constraints on iron spin state at extreme conditions essential for geophysical models of (exo)planetary interiors.
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.
Cu is an ubiquitous material used in industry for its great thermal and electrical properties. Studying the high-pressure high temperature properties of copper (Cu) is relevant for nuclear fusion research as projectiles and flyers used in hypervelocity impacts are generally made of copper, where it is used also in the design of the nuclear fusion targets. Recently, a solid (fcc)-solid (bcc) phase transition has been detected in shock compressed Cu with X-Ray Diffraction. Here, we present a study on shock compressed copper up to 300 GPa and 7100 K probed by single pulse (100 ps FWHM) X-ray Absorption Spectroscopy (XAS). Based on the analysis of the XAS spectra, we provide structural identification and bulk temperature measurements along the Hugoniot up to the melting. The collection of XAS spectra under release conditions, i.e. at later times than the breakout time of the shock wave, helped constraining the experimental fcc-bcc and solid-liquid phase boundaries. In particular, we report the first bulk temperature measurement in shock compressed copper on the melting plateau located between 237(40) GPa and 5750(1130) K and 261 (27) GPa and 6240 (1155) K and on liquid copper at 300 GPa and 7100 K.
Iron(Fe)-water reactions in a magma ocean can influence water storage and density of planets. These reactions can form Fe-O-H phases, whose density, melting, and electronic properties at planetary interior conditions are important for informing planetary models. Here, we study natural goethite (α-FeOOH) that is shock-compressed along its principal Hugoniot. Analysis of our velocity interferometer system for any reflector (VISAR) results extends the equation of state to over 800 GPa. X-ray diffraction and VISAR reflectivity results indicate the onset of melting occurs at 95 GPa with complete melting by 166 GPa, which may be relevant to low seismic velocity anomalies observed above the core-mantle boundary. Analysis of X-ray emission spectroscopy results up to 285 GPa shows the spin crossover of Fe, with dominantly low spin Fe above 265 GPa in the melt, supporting formation of dense basal magma oceans in terrestrial planets. Using our measured FeOOH densities, we model planetary interiors up to 10 Earth masses. Assuming FeOOH forms via iron-water reactions, the radius decreases by up to 28
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.
Laser-driven dynamic compression experiments of plastic materials have found surprisingly fast formation of nanodiamonds (ND) via X-ray probing. This mechanism is relevant for planetary models, but could also open efficient synthesis routes for tailored NDs. We investigate the release mechanics of compressed NDs by molecular dynamics simulation of the isotropic expansion of finite size diamond from different P-T states. Analysing the structural integrity along different release paths via molecular dynamic simulations, we found substantial disintegration rates upon shock release, increasing with the on-Hugnoiot shock temperature. We also find that recrystallization can occur after the expansion and hence during the release, depending on subsequent cooling mechanisms. Our study suggests higher ND recovery rates from off-Hugoniot states, e.g., via double-shocks, due to faster cooling. Laser-driven shock compression experiments of polyethylene terephthalate (PET) samples with in situ X-ray probing at the simulated conditions found diamond signal that persists up to 11 ns after breakout. In the diffraction pattern, we observed peak shifts, which we attribute to thermal expansion of the NDs and thus a total release of pressure, which indicates the stability of the released NDs.
Molten silicates existing at depth play an important role in planetary evolution. Yet, understanding the local structure and properties of liquid silicates under extreme pressure and temperature remains challenging due to the inherent complexities of experimental measurements in such conditions and to the theoretical challenges caused to atomistic simulations by the description of Fe atom behavior. In this presentation, we will show recent results obtained by coupling laser-driven dynamic compression to in situ X-ray probes at the MEC end-station of LCLS at SLAC (Menlo Park, CA, USA) and at the ID24-HPLF instrument at the ESRF (Grenoble, France). The combination of the ultrabright X-ray sources and high-power optical lasers allowed us to probe the local atomic arrangement, spin-state and insights on the electronic structure of shock compressed liquid (Mg,Fe)SiO3 and other Fe-bearing compositions up to 400 GPa along their Hugoniot.
Studying the properties and phase diagram of iron at high-pressure and high-temperature conditions has relevant implications for Earth's inner structure and dynamics and the temperature of the inner core boundary (ICB) at 330 GPa. Also, a hexagonal-closed packed to body-centered cubic (bcc) phase transition has been predicted by many theoretical works but observed only in a few experiments. The recent coupling of high-power laser with advanced x-ray sources from synchrotrons allows for novel approaches to address these issues. Here, we present a study on shock compressed iron up to 270 GPa and 5800 K probed by single-pulse (100 ps FWHM) x-ray absorption spectroscopy (XAS). Based on the analysis of the XAS spectra, we provide structural identification and bulk temperature measurements along the Hugoniot up to the melting. These results rule out the predicted transition to a high-temperature bcc phase and allow one to discriminate among existing equations of state models and melting curves. In particular, we report the first bulk temperature measurement in shock compressed iron on the melting plateau at 240(20) GPa and 5345 (600) K. The melting curve resulting from our work extrapolates to a temperature of 6202(514) K at 330 GPa and represents a refined upper bound for the ICB temperature.
Molten silicates at depth are crucial for planetary evolution, yet their local structure and physical properties under extreme conditions remain elusive due to experimental challenges. In this study, we utilize in situ X-ray diffraction (XRD) at the Matter in Extreme Conditions (MEC) end-station of the Linear Coherent Linac Source (LCLS) at SLAC National Accelerator Laboratory to investigate liquid silicates. Using an ultrabright X-ray source and a high-power optical laser, we probed the local atomic arrangement of shock-compressed liquid (Mg,Fe)SiO3 with varying Fe content, at pressures from 81(9) to 385(40) GPa. We compared these findings to ab initio molecular dynamics simulations under similar conditions. Results indicate continuous densification of the O-O and Mg-Si networks beyond Earth’s interior pressure range, potentially altering melt properties at extreme conditions. This could have significant implications for early planetary evolution, leading to notable differences in differentiation processes between smaller rocky planets, such as Earth and Venus, and super-Earths, which are exoplanets with masses nearly three times that of Earth. Combining laser-driven shock compression and ultra-short X-ray pulses from LCLS, the local structure of liquid silicates was determined up to 385 GPa. Compared with molecular dynamics calculations, continuous densification of O-O and Mg-Si networks may alter melt properties and impact planetary differentiation.
We demonstrate a significantly simplified experimental approach for investigating liquid metallic hydrogen, which is crucial to understand the internal structure and evolution of giant planets. Plastic samples were shock-compressed and then probed by short pulses of X-rays generated by free electron lasers. By comparison with ab initio simulations, we provide indirect evidence for the creation of elemental hydrogen in shock-compressed plastics at -150 GPa and -5, 000 K and thus in a regime where hydrogen is predicted to be metallic. Being the most common form of condensed matter in our solar system, and ostensibly the simplest of all elements, hydrogen is the model case for many theoretical studies and we provide a new possibility to benchmark models for conditions with extreme pressures and temperatures. Moreover, this approach will also allow to probe the chemical behavior of metallic hydrogen in mixture with other elements, which, besides its importance for planetary physics, may open up promising pathways for the synthesis of new materials.
This work presents first insights into the dynamics of free-surface release clouds from dynamically compressed polystyrene and pyrolytic graphite at pressures up to 200 GPa, where they transform into diamond or lonsdaleite, respectively. These ejecta clouds are released into either vacuum or various types of catcher systems, and are monitored with high-speed recordings (frame rates up to 10 MHz). Molecular dynamics simulations are used to give insights to the rate of diamond preservation throughout the free expansion and the catcher impact process, highlighting the challenges of diamond retrieval. Raman spectroscopy data show graphitic signatures on a catcher plate confirming that the shock-compressed PS is transformed. First electron microscopy analyses of solid catcher plates yield an outstanding number of different spherical-like objects in the size range between ten(s) up to hundreds of nanometres, which are one type of two potential diamond candidates identified. The origin of some objects can unambiguously be assigned, while the history of others remains speculative.
The Streaked Optical Pyrometer (SOP) is a visible diagnostic widely used to study the warm dense matter regime at high energy laser facilities, gas guns, or ion accelerators. It is usually coupled with a Velocity Interferometer System for Any Reflector (VISAR) diagnostic for simultaneous shock wave velocity, reflectivity, and temperature measurements to study the Equation of State (EOS) of materials. While VISAR is a well-mastered technology that provides velocity measurements with low relative uncertainties (close to percent), SOP diagnostics still suffer from high imprecision. In this article, we present a new calibration method in order to obtain absolute temperature measurements with reduced uncertainties. This approach is based on a novel light source: a Ce:YAG luminescent concentrator pumped by LEDs. This device produces enough optical power for calibration at the nanosecond sweep duration of the streak camera. As a demonstration, it has first been installed at the LULI facility and tested on quartz samples shocked at temperatures above 4000 K.
In this study, we investigated phase transformations of CaTiO3 perovskite using x-ray diffraction at high pressure and high temperature up to 170 GPa and 4500 K in a laser-heated diamond-anvil cell. We report a high-pressure dissociation of CaTiO3 into CaO-B2 and CaTi2O5 with a monoclinic P2/m structure, instead of the expected transformation of the orthorhombic distorted perovskite structure into a post-perovskite phase. We propose that this transition may be favored by the B1 to B2 phase change of CaO at around 60 GPa. In order to provide additional information on the high pressure properties of CaTiO3 perovskite, we measured its melting temper-ature using CO2 laser heated diamond anvil cell up to 55 GPa yielding a fit of the melting curve to a Kraut-Kennedy empirical law according to: Tm (K) = 2188 * [1 + 4.23 * (Delta V/V0)]. To provide some further insight into the thermodynamic properties of CaTiO3, we determined the P-V-T equation of state of the orthorhombic mineral perovskite, fitted by using a third order Birch-Murnaghan equation of state and a Berman thermal expansion model. The fit of the data yields to K0 = 180.6(4) GPa, K ' 0 = 4 (fixed), partial differential K/ partial differential T =-0.022(1) GPa K-1, alpha 1 = 3.25(5) x 10-5 K-1, alpha 2 = 1.3(1) x 10-8 K-2
Under high pressures and temperatures, molecular systems with substantial polarization charges, such as ammonia and water, are predicted to form superionic phases and dense fluid states with dissociating molecules and high electrical conductivity. This behaviour potentially plays a role in explaining the origin of the multipolar magnetic fields of Uranus and Neptune, whose mantles are thought to result from a mixture of H 2 O, NH 3 and CH 4 ices. Determining the stability domain, melting curve and electrical conductivity of these superionic phases is therefore crucial for modelling planetary interiors and dynamos. Here we report the melting curve of superionic ammonia up to 300 GPa from laser-driven shock compression of pre-compressed samples and atomistic calculations. We show that ammonia melts at lower temperatures than water above 100 GPa and that fluid ammonia’s electrical conductivity exceeds that of water at conditions predicted by hot, super-adiabatic models for Uranus and Neptune, and enhances the conductivity in their fluid water-rich dynamo layers.
We calculate reflectivities of dynamically compressed water, water-ethanol mixtures, and ammonia at infrared and optical wavelengths with density functional theory and molecular dynamics simulations. The influence of the exchange-correlation functional on the results is examined in detail. Our findings indicate that the consistent use of the HSE hybrid functional reproduces experimental results much better than the commonly used PBE functional. The HSE functional offers not only a more accurate description of the electronic band gap but also shifts the onset of molecular dissociation in the molecular dynamics simulations to significantly higher pressures. We also highlight the importance of using accurate reference standards in reflectivity experiments and reanalyze infrared and optical reflectivity data from recent experiments. Thus, our combined theoretical and experimental work explains and resolves lingering discrepancies between calculations and measurements for the investigated molecular substances under shock compression.
LED-pumped Luminescent Concentrator (LC) has already demonstrated its performance to pump transition metal lasers [1]. This incoherent source of high brightness and high optical power can also be useful for direct emission instead of laser pumping [2]. As an example, absolute calibration of streak cameras requires high optical power over the short sweep duration (from few ns to hundreds of ns). To date, traditional sources like spectral lamps, halogens or even LEDs are not bright and powerful enough for this calibration. In this work, we demonstrate that a LED-pumped Ce:YAG luminescent concentrator is able to calibrate a streaked optical pyrometer (SOP) dedicated to temperature measurements of plasmas on high-energy laser facilities.
The spin state of Fe can alter the key physical properties of silicate melts, affecting the early differentiation and the dynamic stability of the melts in the deep rocky planets. The low-spin state of Fe can increase the affinity of Fe for the melt over the solid phases and the electrical conductivity of melt at high pressures. However, the spin state of Fe has never been measured in dense silicate melts due to experimental challenges. We report detection of dominantly low-spin Fe in dynamically compressed olivine melt at 150 to 256 gigapascals and 3000 to 6000 kelvin using laser-driven shock wave compression combined with femtosecond x-ray diffraction and x-ray emission spectroscopy using an x-ray free electron laser. The observation of dominantly low-spin Fe supports gravitationally stable melt in the deep mantle and generation of a dynamo from the silicate melt portion of rocky planets.
Angularly resolved X-ray scattering measurements from fs-laser heated hydrogen have been used to determine the equilibration of electron and ion temperatures in the warm dense matter regime. The relaxation of rapidly heated cryogenic hydrogen is visualized using 5.5 keV X-ray pulses from the Linac Coherent Light (LCLS) source in a 1 Hz repetition rate pump-probe setting. We demonstrate that the electron-ion energy transfer is faster than quasi-classical Landau-Spitzer models that use ad hoc cutoffs in the Coulomb logarithm.
Carbonate minerals, for example calcite and magnesite, exist on the planetary surfaces of the Earth, Mars, and Venus, and are subjected to hypervelocity collisions. The physical properties of planetary materials at extreme conditions are essential for understanding their dynamic behaviors at hypervelocity collisions and the mantle structure of rocky planets including Super-Earths. Here we report laboratory investigations of laser-shocked calcite at pressures of 200-960 GPa (impact velocities of 12-30 km/s and faster than escape velocity from the Earth) using decay shock techniques. Our measured temperatures above 200 GPa indicated a large difference from the previous theoretical models. The present shock Hugoniot data and temperature measurements, compared with the previous reports, indicate melting without decomposition at pressures of ~110 GPa to ~& nbsp;350 GPa and a bonded liquid up to 960 GPa from the calculated specific heat. Our temperature calculations of calcite at 1 atm adiabatically released from the Hugoniot points suggest that the released products vary depending on the shock pressures and affect the planetary atmosphere by the degassed species. The present results on calcite newly provide an important anchor for considering the theoretical EOS at the extreme conditions, where the model calculations show a significant diversity at present.