arXiv subjects

J. S. Wark

Publications and source records attributed to J. S. Wark.

17 recordsLinked to original sources

arXiv2026

Nanosecond timescale plasticity in shock-compressed polycrystalline MgO: evidence for transition in mechanism above 100 GPa

The mechanical properties of ceramics under extreme conditions directly impact applications ranging from shielding spacecrafts, designing plasma facing materials in nuclear fusion to understanding the rheology of deep planetary interiors. Here, we use polycrystalline MgO as a model ceramic to understand the high-pressure-temperature mechanical behaviour of such materials under extreme strain rates. We use laser-driven shock compression up to 175(15) GPa on the principal Hugoniot along with ultrafast diagnostics at the European X-ray Free Electron Laser to probe the dominant deformation mechanisms with changing P -T conditions. These near-instantaneous time-resolved snapshots, coupled with elasto-viscoplastic self-consistent (EVPSC) simulations, strongly suggest that MgO attains plastic regime in the nanoseconds scale accompanied by a pressure-mediated change in dominant slip system between 95 and 175 GPa. This work provides a new direct window into the deformation dynamics of polycrystalline ceramics under high-velocity impacts.

cond-mat.mtrl-sci↗

arXiv2026

Ultrafast temperature diagnosis of dynamically compressed matter using millielectronvolt inelastic x-ray scattering beyond the first Brillouin zone

We present calculations of the millielectronvolt-scale x-ray scattering spectra of multilayered dynamic-compression targets comprising an unstructured ablator layer and a crystalline, textured sample layer. Our model builds on the classic formulation of x-ray thermal diffuse scattering by Warren [B. E. Warren, Acta Crystallogr. 6, 803 (1953)] and includes both elastic and first-order (single-phonon) inelastic scattering contributions to the dynamic structure factor $S(\mathbf{q},ω)$. We focus on the umklapp scattering regime (i.e., at momentum transfers outside the first Brillouin zone) where the ablator scattering that threatens to overwhelm the inelastic scattering from the crystalline layer of interest is suppressed. We show that, despite the considerably more complex structure of the inelastic scattering spectra in this intermediate-$q$ regime, it is still possible to reliably deduce the temperature of the crystal using Dornheim's Laplace-transform--based formalism [Dornheim et al., Phys. Plasmas 30, 042707 (2023)], regardless of the details of the sample's texture.

physics.app-ph↗

arXiv2025

X-ray thermal diffuse scattering as a texture-robust temperature diagnostic for dynamically compressed solids

We present a model of x-ray thermal diffuse scattering (TDS) from a cubic polycrystal with an arbitrary crystallographic texture, based on the classic approach of Warren. We compare the predictions of our model with femtosecond x-ray diffraction patterns obtained from ambient and dynamically compressed rolled copper foils obtained at the High Energy Density (HED) instrument of the European X-Ray Free-Electron Laser (EuXFEL), and find that the texture-aware TDS model yields more accurate results than does the conventional powder model owed to Warren. Nevertheless, we further show that: with sufficient angular detector coverage, the TDS signal is largely unchanged by sample orientation and in all cases strongly resembles the signal from a perfectly random powder; shot-to-shot fluctuations in the TDS signal resulting from grain-sampling statistics are at the percent level, in stark contrast to the fluctuations in the Bragg-peak intensities (which are over an order of magnitude greater); and TDS is largely unchanged even following texture evolution caused by compression-induced plastic deformation. We conclude that TDS is robust against texture variation, making it a flexible temperature diagnostic applicable just as well to off-the-shelf commercial foils as to ideal powders.

physics.app-ph↗

arXiv2025

Femtosecond temperature measurements of laser-shocked copper deduced from the intensity of the x-ray thermal diffuse scattering

We present 50-fs, single-shot measurements of the x-ray thermal diffuse scattering (TDS) from copper foils that have been shocked via nanosecond laser-ablation up to pressures above 135~GPa. We hence deduce the x-ray Debye-Waller (DW) factor, providing a temperature measurement. The targets were laser-shocked with the DiPOLE 100-X laser at the High Energy Density (HED) endstation of the European X-ray Free-Electron Laser (EuXFEL). Single x-ray pulses, with a photon energy of 18 keV, were scattered from the samples and recorded on Varex detectors. Despite the targets being highly textured (as evinced by large variations in the elastic scattering), and with such texture changing upon compression, the absolute intensity of the azimuthally averaged inelastic TDS between the Bragg peaks is largely insensitive to these changes, and, allowing for both Compton scattering and the low-level scattering from a sacrificial ablator layer, provides a reliable measurement of $T/Θ_D^2$, where $Θ_D$ is the Debye temperature. We compare our results with the predictions of the SESAME 3336 and LEOS 290 equations of state for copper, and find good agreement within experimental errors. We thus demonstrate that single-shot temperature measurements of dynamically compressed materials can be made via thermal diffuse scattering of XFEL radation.

cond-mat.mtrl-sci↗

arXiv2024

Dielectronic satellite emission from a solid-density Mg plasma: relationship to models of ionisation potential depression

We report on experiments where solid-density Mg plasmas are created by heating with the focused output of the Linac Coherent Light Source x-ray free-electron-laser. We study the K-shell emission from the Helium and Lithium-like ions using Bragg crystal spectroscopy. Observation of the dielectronic satellites in Lithium-like ions confirms that the M-shell electrons appear bound for these high charge states. An analysis of the intensity of these satellites indicates that when modelled with an atomic-kinetics code, the ionisation potential depression model employed needs to produce depressions for these ions which lie between those predicted by the well known Stewart-Pyatt and Ecker-Kroll models. These results are largely consistent with recent Density Functional Theory calculations.

hep-ex↗

arXiv2024

Phase transitions of Fe$_2$O$_3$ under laser shock compression

We present in-situ x-ray diffraction and velocity measurements of Fe$_2$O$_3$ under laser shock compression at pressures between 38-116 GPa. None of the phases reported by static compression studies were observed. Instead, we observed an isostructural phase transition from $α$-Fe$_2$O$_3$ to a new $α^\prime$-Fe$_2$O$_3$ phase at a pressure of 50-62 GPa. The $α^\prime$-Fe$_2$O$_3$ phase differs from $α$-Fe$_2$O$_3$ by an 11% volume drop and a different unit cell compressibility. We further observed a two-wave structure in the velocity profile, which can be related to an intermediate regime where both $α$ and $α^\prime$ phases coexist. Density functional theory calculations with a Hubbard parameter indicate that the observed unit cell volume drop can be associated with a spin transition following a magnetic collapse.

cond-mat.mtrl-sci↗

arXiv2021

Atomistic deformation mechanism of silicon under laser-driven shock compression

Silicon (Si) is one of the most abundant elements on Earth, and it is the most important and widely used semiconductor, constituting the basis of modern electronic devices. Despite extensive study, some properties of Si remain elusive. For example, the behaviour of Si under high pressure, in particular at the ultra-high strain rates characteristic of dynamic compression, has been a matter of debate for decades. A detailed understanding of how Si deforms is crucial for a variety of fields, ranging from planetary science to materials design. Simulations suggest that in Si the shear stress generated during shock compression is released inelastically, i.e., via a high-pressure phase transition, challenging the classical picture of relaxation via defect-mediated plasticity. However, experiments at the short timescales characteristic of shock compression are challenging, and direct evidence supporting either deformation mechanism remain elusive. Here, we use sub-picosecond, highly-monochromatic x-ray diffraction to study (100)-oriented single-crystal Si under laser-driven shock compression. We provide the first unambiguous, time-resolved picture of Si deformation at ultra-high strain rates, demonstrating the predicted inelastic shear release. Our results resolve the longstanding controversy on silicon deformation under dynamic compression, and provide direct proof of strain rate-dependent deformation mechanisms in a non-metallic system, which is key for the study of planetary-relevant materials.

cond-mat.mtrl-sci↗

arXiv2021

Crystal plasticity finite element simulation of lattice rotation and x-ray diffraction during laser shock-compression of Tantalum

Wehrenberg et. al. [Nature 550 496 (2017)] used ultrafast in situ x-ray diffraction at the LCLS x-ray free-electron laser facility to measure large lattice rotations resulting from slip and deformation twinning in shock-compressed laser-driven [110] fibre textured tantalum polycrystal. We employ a crystal plasticity finite element method model, with slip kinetics based closely on the isotropic dislocation-based Livermore Multiscale Model [Barton et. al., J. Appl. Phys. 109 (2011)], to analyse this experiment. We elucidate the link between the degree of lattice rotation and the kinetics of plasticity, demonstrating that a transition occurs at shock pressures of $\sim$27 GPa, between a regime of relatively slow kinetics, resulting in a balanced pattern of slip system activation and therefore relatively small net lattice rotation, and a regime of fast kinetics, due to the onset of nucleation, resulting in a lop-sided pattern of deformation-system activation and therefore large net lattice rotations. We demonstrate a good fit between this model and experimental x-ray diffraction data of lattice rotation, and show that this data is constraining of deformation kinetics.

cond-mat.mtrl-sci↗

arXiv2020

Mapping the Electronic Structure of Warm Dense Nickel via Resonant Inelastic X-ray Scattering

The development of high-brightness free-electron lasers (FEL) has revolutionised our ability to create and study matter in the high-energy-density (HED) regime. Current diagnostic techniques have been very successful in yielding information on fundamental thermodynamic plasma properties, but provide only limited or indirect information on the detailed quantum structure of these systems, and on how it is affected by ionization dynamics. Here we show how the electronic structure of solid-density nickel, heated to temperatures of 10's of eV on femtosecond timescales, can be studied by resonant (Raman) inelastic x-ray scattering (RIXS) using the Linac Coherent Light Source FEL. We present single-shot measurements of the valence density of states in the x-ray-heated transient system, and extract simultaneously electron temperatures, ionization, and ionization potential energies. The RIXS spectrum provides a wealth of information on the valence structure of the HED system that goes beyond what can be extracted from x-ray absorption or emission spectroscopy alone.

physics.plasm-ph↗

arXiv2020

Time-resolved XUV Opacity Measurements of Warm-Dense Aluminium

The free-free opacity in plasmas is fundamental to our understanding of energy transport in stellar interiors and for inertial confinement fusion research. However, theoretical predictions in the challenging dense plasma regime are conflicting and there is a dearth of accurate experimental data to allow for direct model validation. Here we present time-resolved transmission measurements in solid-density Al heated by an XUV free-electron laser. We use a novel functional optimization approach to extract the temperature-dependent absorption coefficient directly from an oversampled pool of single-shot measurements, and find a pronounced enhancement of the opacity as the plasma is heated to temperatures of order the Fermi energy. Plasma heating and opacity-enhancement is observed on ultrafast time scales, within the duration of the femtosecond XUV pulse. We attribute further rises in the opacity on ps timescales to melt and the formation of warm-dense matter.

physics.plasm-ph↗

arXiv2018

Ab-initio simulations and measurements of the free-free opacity in Aluminum

The free-free opacity in dense systems is a property that both tests our fundamental understanding of correlated many-body systems, and is needed to understand the radiative properties of high energy-density plasmas. Despite its importance, predictive calculations of the free-free opacity remain challenging even in the condensed matter phase for simple metals. Here we show how the free-free opacity can be modelled at finite-temperatures via time-dependent density functional theory, and illustrate the importance of including local field corrections, core polarization and self-energy corrections. Our calculations for ground-state Al are shown to agree well with experimental opacity measurements performed on the Artemis laser facility across a wide range of x-ray to ultraviolet wavelengths. We extend our calculations across the melt to the warm-dense matter regime, and find good agreement with advanced plasma models based on inverse bremsstrahlung at temperatures above 10 eV.

physics.plasm-ph↗

arXiv2018

Validating Continuum Lowering Models via Multi-Wavelength Measurements of Integrated X-ray Emission

X-ray emission spectroscopy is a well-established technique used to study continuum lowering in dense plasmas. It relies on accurate atomic physics models to robustly reproduce high-resolution emission spectra, and depends on our ability to identify spectroscopic signatures such as emission lines or ionization edges of individual charge states within the plasma. Here we describe a method that forgoes these requirements, enabling the validation of different continuum lowering models based solely on the total intensity of plasma emission in systems driven by narrow-bandwidth x-ray pulses across a range of wavelengths. The method is tested on published Al spectroscopy data and applied to the new case of solid-density partially-ionized Fe plasmas, where extracting ionization edges directly is precluded by the significant overlap of emission from a wide range of charge states.

physics.plasm-ph↗

arXiv2013

Direct measurement of time-dependent density-density correlations in a solid through the acoustic analog of the dynamical Casimir effect

The macroscopic characteristics of a solid, such as its thermal, optical or transport properties are determined by the available microscopic states above its lowest energy level. These slightly higher quantum states are described by elementary excitations and dictate the response of the system under external stimuli. The spectrum of these excitations, obtained typically from inelastic neutron and x-ray scattering, is the spatial and temporal Fourier transform of the density-density correlation function of the system, which dictates how a perturbation propagates in space and time. As frequency-domain measurements do not generally contain phase information, time-domain measurements of these fluctuations could yield a more direct method for investigating the excitations of solids and their interactions both in equilibrium and far-from equilibrium. Here we show that the diffuse scattering of femtosecond x-ray pulses produced by a free electron laser (FEL) can directly measure these density-density correlations due to lattice vibrations in the time domain. We obtain spectroscopic information of the lattice excitations with unprecedented momentum- and frequency- resolution, without resolving the energy of the outgoing photon. Correlations are created via an acoustic analog of the dynamical Casimir effect, where a femtosecond laser pulse slightly quenches the phonon frequencies, producing pairs of squeezed phonons at momenta +q and -q. These pairs of phonons manifest as macroscopic, time-dependent coherences in the displacement correlations that are then probed directly by x-ray scattering. Since the time-dependent correlations are preferentially created in regions of strong electron-phonon coupling, the time-resolved approach is natural as a spectroscopic tool of low energy collective excitations in solids, and their microscopic interactions, both in linear response and beyond.

cond-mat.mtrl-sci↗

arXiv2009

XUV Opacity of Aluminum between the Cold-Solid to Warm-Plasma Transition

We present calculations of the free-free XUV opacity of warm, solid-density aluminum at photon energies between the plasma frequency at 15 eV and the L-edge at 73 eV, using both density functional theory combined with molecular dynamics and a semi-analytical model in the RPA framework with the inclusion of local field corrections. As the temperature is increased from room temperature to 10 eV, with the ion and electron temperatures equal, we calculate an increase in the opacity in the range over which the degree of ionization is constant. The effect is less pronounced if only the electron temperature is allowed to increase. The physical significance of these increases is discussed in terms of intense XUV-laser matter interactions on both femtosecond and picosecond time-scales.

physics.plasm-ph↗

arXiv2008

Line intensity enhancements in stellar coronal X-ray spectra due to opacity effects

Context. The I(15.01 A)/I(16.78 A) emission line intensity ratio in Fe XVII has been reported to deviate from its theoretical value in solar and stellar X-ray spectra. This is attributed to opacity in the 15.01 A line, leading to a reduction in its intensity, and was interpreted in terms of a geometry in which the emitters and absorbers are spatially distinct. Aims. We study the I(15.01 A)/I(16.78 A) intensity ratio for the active cool dwarf EV Lac, in both flare and quiescent spectra. Methods. The observations were obtained with the Reflection Grating Spectrometer on the XMM-Newton satellite. The emission measure distribution versus temperature reconstruction technique is used for our analysis. Results. We find that the 15.01 A line exhibits a significant enhancement in intensity over the optically thin value. To our knowledge, this is the first time that such an enhancement has been detected on such a sound statistical basis. We interpret this enhancement in terms of a geometry in which the emitters and absorbers are not spatially distinct, and where the geometry is such that resonant pumping of the upper level has a greater effect on the observed line intensity than resonant absorption in the line-of-sight.

astro-ph↗

arXiv2005

Simulations of Time-Resolved X-Ray Diffraction in Laue Geometry

A method of computer simulation of Time-Resolved X-ray Diffraction (TRXD) in asymmetric Laue (transmission) geometry with an arbitrary propagating strain perpendicular to the crystal surface is presented. We present two case studies for possible strain generation by short-pulse laser irradiation: (i) a thermoelastic-like analytic model; (ii) a numerical model including effects of electron-hole diffusion, Auger recombination, deformation potential and thermal diffusion. A comparison with recent experimental results is also presented.

cond-mat.mtrl-sci↗

arXiv2002

Supersonic strain front driven by a dense electron-hole plasma

We study coherent strain in (001) Ge generated by an ultrafast laser-initiated high density electron-hole plasma. The resultant coherent pulse is probed by time-resolved x-ray diffraction through changes in the anomalous transmission. The acoustic pulse front is driven by ambipolar diffusion of the electron-hole plasma and propagates into the crystal at supersonic speeds. Simulations of the strain including electron-phonon coupling, modified by carrier diffusion and Auger recombination, are in good agreement with the observed dynamics.

cond-mat.mtrl-sci↗