arXiv subjects

Justin S. Wark

Publications and source records attributed to Justin S. Wark.

14 recordsLinked to original sources

arXiv2026

A Momentum-Resolved X-ray Thomson Scattering Benchmark of Electronic-Response Models in Warm Dense Aluminium

The robust diagnosis of conditions generated in warm dense matter (WDM) experiments remains a persistent challenge. Here we describe the measurement of shock-compressed aluminium at 50 GPa with angle-resolved femtosecond x-ray Thomson scattering (XRTS) over a wide range of scattering wavevectors at the European XFEL. The measured plasmon dispersion and line shape show that the de facto standard approach for analysing XRTS spectra, based on uniform-electron-gas models, systematically overestimates the resonance energy by up to 8 eV. We present an ab initio approach that agrees within the experimental uncertainty and demonstrates that accounting for shock-induced disorder is critical for interpreting shock-compressed systems, providing evidence that ab initio treatments are required for reliable XRTS inference in warm dense aluminium.

physics.plasm-ph↗

arXiv2025

Structural evolution of iron oxides melts at Earth's outer-core pressures

Oxygen and other light elements comprise up to 5 wt% of the Earth's outer-core, and may significantly influence its physical properties and the operation of the geodynamo. Here we report in situ x-ray diffraction measurements of Fe, Fe + 4.5 FeO (atomic proportion), and Fe2O3 melts at 177-438 GPa, achieved using laser-driven shock compression at an x-ray free-electron laser. The melts exhibit Fe-O coordination numbers between 4.0(0.4) and 4.5(0.4), indicating predominantly four-fold coordination environments. These coordination states are significantly smaller than those of Fe-bearing lower-mantle phases such as bridgmanite and ferropericlase. Shorter Fe-Fe interatomic distances in compressed iron oxide melts drive the denser packing relative to ambient melts, while the structural differences between Fe + 4.5 FeO and Fe2O3 melts under shock indicate that the oxidation state modulates oxygen solubility in liquid Fe. At around 177 GPa (380 km below the core-mantle boundary), Fe2O3 melts exhibit higher Fe-O coordination, suggesting that local variations in oxygen content could contribute to the stratification in the uppermost outer-core inferred from seismological and geomagnetic observations.

cond-mat.mtrl-sci↗

arXiv2024

Shock-driven amorphization and melt in Fe$_2$O$_3$

We present measurements on Fe$_2$O$_3$ amorphization and melt under laser-driven shock compression up to 209(10) GPa via time-resolved in situ x-ray diffraction. At 122(3) GPa, a diffuse signal is observed indicating the presence of a non-crystalline phase. Structure factors have been extracted up to 182(6) GPa showing the presence of two well-defined peaks. A rapid change in the intensity ratio of the two peaks is identified between 145(10) and 151(10) GPa, indicative of a phase change. Present DFT+$U$ calculations of temperatures along Fe$_2$O$_3$ Hugoniot are in agreement with SESAME 7440 and indicate relatively low temperatures, below 2000 K, up to 150 GPa. The non-crystalline diffuse scattering is thus consistent with the - as yet unreported - shock amorphization of Fe$_2$O$_3$ between 122(3) and 145(10) GPa, followed by an amorphous-to-liquid transition above 151(10) GPa. Upon release, a non-crystalline phase is observed alongside crystalline $α$-Fe$_2$O$_3$. The extracted structure factor and pair distribution function of this release phase resemble those reported for Fe$_2$O$_3$ melt at ambient pressure.

cond-mat.mtrl-sci↗

arXiv2024

Exploring relaxation dynamics in warm dense plasmas by tailoring non-thermal electron distributions with a free electron laser

Knowing the characteristic relaxation time of free electrons in a dense plasma is crucial to our understanding of plasma equilibration and transport. However, experimental investigations of electron relaxation dynamics have been hindered by the ultra-fast, sub-femtosecond time scales on which these interactions typically take place. Here we propose a novel approach that uses x-rays from a free electron laser to generate well-defined non-thermal electron distributions, which can then be tracked via emission spectroscopy from radiative recombination as they thermalize. Collisional radiative simulations reveal how this method can enable the measurement of electron relaxation time scales {\it in situ}, shedding light on the applicability and accuracy of the Coulomb Logarithm framework for modelling collisions in dense plasmas.

physics.plasm-ph↗

arXiv2024

Resonant inelastic x-ray scattering in warm-dense Fe compounds beyond the SASE FEL resolution limit

Resonant inelastic x-ray scattering (RIXS) is a widely used spectroscopic technique, providing access to the electronic structure and dynamics of atoms, molecules, and solids. However, RIXS requires a narrow bandwidth x-ray probe to achieve high spectral resolution. The challenges in delivering an energetic monochromated beam from an x-ray free electron laser (XFEL) thus limit its use in few-shot experiments, including for the study of high energy density systems. Here we demonstrate that by correlating the measurements of the self-amplified spontaneous emission (SASE) spectrum of an XFEL with the RIXS signal, using a dynamic kernel deconvolution with a neural surrogate, we can achieve electronic structure resolutions substantially higher than those normally afforded by the bandwidth of the incoming x-ray beam. We further show how this technique allows us to discriminate between the valence structures of Fe and Fe$_2$O$_3$, and provides access to temperature measurements as well as M-shell binding energies estimates in warm-dense Fe compounds.

cond-mat.mtrl-sci↗

arXiv2023

Quantifying ionization in hot dense plasmas

Ionization is a problematic quantity in that it does not have a well-defined thermodynamic definition, yet it is a key parameter within plasma modelling. One still therefore aims to find a consistent and unambiguous definition for the ionization state. Within this context we present finite-temperature density functional theory calculations of the ionization state of carbon in CH plasmas using two potential definitions: one based on counting the number of continuum electrons, and another based on the optical conductivity. Differences of up to 10\% are observed between the two methods. However, including "Pauli forbidden" transitions in the conductivity reproduces the counting definition, suggesting such transitions are important to evaluate the ionization state.

physics.plasm-ph↗

arXiv2023

Investigating Mechanisms of State Localization in Highly-Ionized Dense Plasmas

We present the first experimental observation of K$_β$ emission from highly charged Mg ions at solid density, driven by intense x-rays from a free electron laser. The presence of K$_β$ emission indicates the $n=3$ atomic shell is relocalized for high charge states, providing an upper constraint on the depression of the ionization potential. We explore the process of state relocalization in dense plasmas from first principles using finite-temperature density functional theory alongside a wavefunction localization metric, and find excellent agreement with experimental results.

physics.plasm-ph↗

arXiv2023

Simulations of Collisional Effects in an Inner-Shell Solid-Density Mg X-Ray Laser

Inner-shell K$α$ x-ray lasers have been created by pumping gaseous, solid, and liquid targets with the intense x-ray output of free-electron-lasers (FELs). For gaseous targets lasing relies on the creation of K-shell core-holes on a time-scale short compared with filling via Auger decay. In the case of solid and liquid density systems, collisional effects will also be important, affecting not only populations, but also line-widths, both of which impact the degree of overall gain, and its duration. However, to date such collisional effects have not been extensively studied. We present here initial simulations using the CCFLY code of inner-shell lasing in solid density Mg, where we self-consistently treat the effects of the incoming FEL radiation and the atomic kinetics of the Mg system, including radiative, Auger, and collisional effects. We find that the combination of collisional population of the lower states of the lasing transitions and broadening of the lines precludes lasing on all but the K$α$ of the initially cold system. Even assuming instantaneous turning on of the FEL pump, we find the duration of the gain in the solid system to be sub-femtosecond.

physics.plasm-ph↗

arXiv2022

Non-thermal evolution of dense plasmas driven by intense x-ray fields

The advent of x-ray free-electron lasers (XFELs) has enabled a range of new experimental investigations into the properties of matter driven to extreme conditions via intense x-ray-matter interactions. The femtosecond timescales of these interactions lead to the creation of transient high-energy-density plasmas, where both the electrons and the ions may be far from local thermodynamic equilibrium (LTE). Predictive modelling of such systems remains challenging because of the substantially different timescales on which electrons and ions thermalize, and because of the vast number of atomic configurations that are required to describe the resulting highly-ionized plasmas. Here we explore the evolution of systems driven to high energy densities using CCFLY, a non-LTE, Fokker-Planck collisional-radiative code. We use CCFLY to investigate the evolution dynamics of a solid-density plasma driven by an XFEL, and explore the relaxation of the plasma to local thermodynamic equilibrium on femtosecond timescales in terms of the charge state distribution, electron density, and temperature.

physics.plasm-ph↗

arXiv2022

Femtosecond Diffraction and Dynamic High Pressure Science

Solid state material at high pressure is prevalent throughout the Universe, and an understanding of the structure of matter under such extreme conditions, gleaned from x-ray diffraction, has been pursued for the best part of a century. The highest pressures that can be reached to date (2 TPa) in combination with x-ray diffraction diagnosis have been achieved by dynamic compression via laser ablation . The past decade has witnessed remarkable advances in x-ray technologies, with novel x-ray Free-Electron-Lasers (FELs) affording the capacity to produce high quality single-shot diffraction data on time scales below 100 fsec. We provide a brief history of the field of dynamic compression, spanning from when the x-ray sources were almost always laser-plasma based, to the current state-of-the art diffraction capabilities provided by FELs. We give an overview of the physics of dynamic compression, diagnostic techniques, and the importance of understanding how the rate of compression influences the final temperatures reached. We provide illustrative examples of experiments performed on FEL facilities that are starting to give insight into how materials deform at ultra-high strain rates, their phase diagrams, and the types of states that can be reached. We emphasize that there often appear to be differences in the crystalline phases observed between use of static and dynamic compression techniques. We give our perspective on both the current state of this rapidly evolving field, and some glimpses of how we see it developing in the near-to-medium term.

cond-mat.other↗

arXiv2022

Slip competition and rotation suppression in tantalum and copper during dynamic uniaxial compression

When compressed, a metallic specimen will generally experience changes to its crystallographic texture due to plasticity-induced rotation. Ultrafast x-ray diffraction techniques make it possible to measure rotation of this kind in targets dynamically compressed over nanosecond timescales to the kind of pressures ordinarily encountered in planetary interiors. The axis and the extent of the local rotation can provide hints as to the combination of plasticity mechanisms activated by the rapid uniaxial compression, thus providing valuable information about the underlying dislocation kinetics operative during extreme loading conditions. We present large-scale molecular dynamics simulations of shock-induced lattice rotation in three model crystals whose behavior has previously been characterized in dynamic-compression experiments: tantalum shocked along its [101] direction, and copper shocked along either [001] or [111]. We find that, in all three cases, the texture changes predicted by the simulations are consistent with those measured experimentally using in situ x-ray diffraction. We show that while tantalum loaded along [101] and copper loaded along [001] both show pronounced rotation due to asymmetric multiple slip, the orientation of copper shocked along [111] is predicted to be stabilized by opposing rotations arising from competing, symmetrically equivalent slip systems.

cond-mat.mtrl-sci↗

arXiv2020

Kinematics of slip-induced rotation for uniaxial shock or ramp compression

When a metallic specimen is plastically deformed, its underlying crystal structure must often rotate in order to comply with its macroscopic boundary conditions. There is growing interest within the dynamic compression community in exploiting x-ray diffraction measurements of lattice rotation to infer which combinations of plasticity mechanisms are operative in uniaxially shock- or ramp-compressed crystals, thus informing materials science at the greatest extremes of pressure and strain rate. However, it is not widely appreciated that several of the existing models linking rotation to slip activity are fundamentally inapplicable to a planar compression scenario. We present molecular dynamics simulations of single crystals suffering true uniaxial strain, and show that the Schmid and Taylor analyses used in traditional materials science fail to predict the ensuing lattice rotation. We propose a simple alternative framework based on the elastoplastic decomposition that successfully recovers the observed rotation for these single crystals, and can further be used to identify the operative slip systems and the amount of activity upon them in the idealized cases of single and double slip.

cond-mat.mtrl-sci↗

arXiv2015

Single Hit Energy-resolved Laue Diffraction

In-situ white light Laue diffraction has been successfully used to interrogate the structure of single crystal materials undergoing rapid (nanosecond) dynamic compression up to megabar pressures. However, information on strain state accessible via this technique is limited, reducing its applicability for a range of applications. We present an extension to the existing Laue diffraction platform in which we record the photon energy of a subset of diffraction peaks. This allows for a measurement of the longitudinal and transverse strains in-situ during compression. Consequently, we demonstrate measurement of volumetric compression of the unit cell, in addition to the limited aspect ratio information accessible in conventional white light Laue. We present preliminary results for silicon, where only an elastic strain is observed. VISAR measurements show the presence of a two wave structure and measurements show that material downstream of the second wave does not contribute to the observed diffraction peaks, supporting the idea that this material may be highly disordered, or has undergone large scale rotation.

cond-mat.mtrl-sci↗

arXiv2015

Simulations of x-ray diffraction from uniaxially-compressed highly-textured polycrystalline targets

A growing number of shock compression experiments, especially those involving laser compression, are taking advantage of in situ x-ray diffraction as a tool to interrogate structure and microstructure evolution. Although these experiments are becoming increasingly sophisticated, there has been little work on exploiting the textured nature of polycrystalline targets to gain information on sample response. Here, we describe how to generate simulated x-ray diffraction patterns from materials with an arbitrary texture function subject to a general deformation gradient. We will present simulations of Debye-Scherrer x-ray diffraction from highly textured polycrystalline targets that have been subjected to uniaxial compression, as may occur under planar shock conditions. In particular, we study samples with a fibre texture, and find that the azimuthal dependence of the diffraction patterns contains information that, in principle, affords discrimination between a number of similar shock-deformation mechanisms. For certain cases we compare our method with results obtained by taking the Fourier Transform of the atomic positions calculated by classical molecular dynamics simulations. Illustrative results are presented for the shock-induced $α$-$ε$ phase transition in iron, the $α$-$ω$ transition in titanium and deformation due to twinning in tantalum that is initially preferentially textured along [001] and [011]. The simulations are relevant to experiments that can now be performed using 4th generation light sources, where single-shot x-ray diffraction patterns from crystals compressed via laser-ablation can be obtained on timescales shorter than a phonon period.

cond-mat.mtrl-sci↗